Mother Margaret Mary Brady held several administrative positions in the Sisters of St. Joseph community before to becoming president of the Mount. It was during her term as provincial superior in June 1925 that she responded to Bishop Cantwell's request to establish a Catholic women’s college in Los Angeles. The first student entered that same fall. During her presidency she oversaw construction of the “College Building” on the St. Mary's Academy campus and selected a hilltop in Brentwood for a permanent site. In spite of sparse finances and the Great Depression, she saw to the successful construction of the first building at Chalon, now called Brady Hall, which the College occupied in 1930. She also launched the 12-year process of raising funds for the future Mary Chapel. Today, the annual Brady Award is given to a student who entered Mount St. Mary's later in life.
Mother Dolorosa Mannix served as the Mount's first dean until she was appointed president and CSJ provincial in 1937. She brought in several new faculty members - sisters, priests, brothers and laypersons - to strengthen the arts, sciences, and education curricula. Despite the Depression, Mother Dolorosa was finally able to finance the construction of Mary Chapel, which was dedicated on May 2, 1940 - nearly 10 years after its planned opening. Rossiter Hall, the residence for the teaching sisters, followed in 1944. By the time Sister stepped down as president, the Mount was debt-free. After completing her six-year term in 1943 she continued to teach until 1958. The Alumnae Association continues to honor her with the annual Sister Dolorosa Alumnae Award, given to an outstanding baccalaureate graduate.
As CSJ superior and the Mount's third president, Mother Marie de Lourdes Le May brought with her a background in English literature. During her presidency the college became fully accredited to grant elementary and junior high credentials. The draw of these prestigious programs and a growing student population required a new construction. Overcoming wartime rationing in building materials, the Mount built St. Joseph Hall in 1944 with new science labs, classrooms, theater and administrative offices. That same year Mother Marie de Lourdes purchased 21.7 acres, increasing the Chalon Campus to close to the present size. In 1946, the Charles Willard Coe Memorial Library was built with funds left to Sister Celine Coe, CSJ, by her rancher father. Mother Marie de Lourdes also launched the campus newspaper The View, The Mount yearbook and Alumnae Echoes newsletter.
Mother Agnes Marie O'Loughlin, the Mount's forth president and religious superior, presided over the College's 25th anniversary in 1950. She added several new departments: education, drama, physical education, and a unique cancer research curriculum, the only known program of its kind at the time. She fostered increased faculty participation in decision-making. Most significant, the Mount's renowned bachelor's program in nursing was launched in 1948, the first baccalaureate nursing program in California. In 1953, the Mount joined with 10 other colleges to form the Independent Colleges of Southern California (ICSC). A family trust in Sister Agnes Marie's name continues to support the Mount.
Mother Rosemary Lyons, the fifth president, served only three years but oversaw many changes to the Chalon Campus. She negotiated the complex financing to construct Carondelet Hall, the Mount's first dedicated dormitory. Setting the stage for the eventual Doheny program, Mother Rosemary opened an off-campus center in the mid-1950s in Downtown Los Angeles on the estate of the Doheny Family, primarily for CSJs teaching in the area and working on their degrees. The Los Angeles CSJ province was growing rapidly, and in 1955, the College got a new neighbor, Carondelet Center, then known as the House of Studies. The increased CSJ responsibilities along with the presidency led the Province to divide the job. Sister Rosemary remained Provincial for the full six-year term.
A Mount alumna and member of the College's second graduating class, Sister Rose Gertrude Calloway had experience as dean, director of residence, and chair of the mathematics department. She immediately formed a board of administrators, faculty, and staff to oversee the internal administration of the College and to interact with the board of trustees, faculty and students. When Countess Estelle Doheny passed away in October 1958 the Doheny estate was left to the Catholic Archdiocese of Los Angeles. Sister Rose Gertrude negotiated with Cardinal McIntyre to assume ownership of several of the Victorian mansions for use by the CSJs and College. Like her predecessors, Sister Rose Gertrude returned to teaching after her term was completed, and worked as a volunteer around the campus for many years after retirement.
When Sister Rebecca Doan became the seventh president of Mount St. Mary's College, the role of the religious superior and president were again combined. On December 4, 1961, Sister Rebecca announced publicly that the college would offer an innovative two-year associate in arts degree program beginning in September 1962 on the new Downtown Campus. It was to be the first Catholic college on the West Coast to offer an A.A. degree. But before Sister Rebecca could give her full attention to the new program, she had to focus on an unexpected disaster. The Bel Air fire of November 6, 1961, destroyed one-fifth of the Chalon Campus and part of Carondelet Center. Early the following year she announced a $10-million long range development plan, known as SPACE (Scholastic and Physical Advancement Centered on Excellence) to raise money for expansion of both campuses. In 1965 the Humanities Building added much-needed classroom space at Chalon, and a new classroom building and auditorium became first new construction at Chester Place since the early 20th Century. The Sister Rebecca Doan Award is given to an outstanding graduate who began her career at Doheny.
As Sister Cecilia Louise Moore, a Mount alumna, began her presidency, Mount St. Mary's College was starting to reflect some of the significant changes occurring in society, higher education, and the post-Vatican II Church. Realizing the need to reinforce the College's mission in light of the change, she worked to adapt the Mount to these new realities. Known as "C.L.," Sister Cecilia Louise created two new advisory bodies and several new positions, adding to the number of lay persons filling these positions. The rapidly changing demographics of Los Angeles led her to create support programs for students to improve their English and academic skills. The Women's Leadership program followed in 1975. Completing the strategic plan for the Doheny Campus, Sister Cecilia Louise negotiated with Cardinals McIntyre and Manning for title to the remaining Doheny property, giving the Mount both sides of Chester Place and a strong plan for the future.
The Mount began its second 50 years with Sister Magdalen Coughlin as president. The 1970s and 1980s brought a steady increase in ethnic and cultural diversity in Los Angeles, but also growing numbers of academically under-prepared students to the Mount. Seeing education as an investment in the future leadership of California and the nation, Sister Magdalen led the College in a period of broad innovation, training faculty in multicultural pedagogy, developing new courses and requirements and earning the Mount a national reputation for its work with diverse student bodies. She oversaw the construction of a new dormitory and Mercy Chapel at Doheny. In 1989 she stepped into the position of Chancellor and was an active fundraiser at the time of her death in 1994.
Sister Karen M. Kennelly, the 10th president of Mount St. Mary's College, was the first CSJ from outside of the Los Angeles Province. She championed the College's initiatives in diversity and embarked on an ambitious program to upgrade technology on both campuses. Central to this effort was the extensive renovation of the Charles Willard Coe Memorial Library in 1995 and the construction of the Sister Magdalen Coughlin Learning Complex at Doheny, which included a completely new library named for Mount benefactor J. Thomas McCarthy. One of Sister Karen's first affirmations as president came in 1990 from U.S. News & World Report when, for the first time, the Mount ranked among the top liberal art colleges in the West, an honor that was repeated throughout her presidency. The Mount's outreach to nontraditional students took on its current form in 1992 with the establishment of Weekend College, and the nursing programs were expanded in response to growing demand for healthcare professionals.
Jacqueline Powers Doud became the eleventh president of Mount St. Mary's College on July 1, 2000. She served MSMC as provost and vice president for academic affairs before becoming the College's first lay president. She had more than 30 years of experience in senior administration, serving the University of La Verne, Woodbury University, and Mount St. Mary's, following nine years of teaching experience in French, humanities and education. In 2010, Cardinal Roger Mahony honored Doud with the Cardinal's Award of the Los Angeles Archdiocese. New academic programs launched during Dr. Doud's tenure included an expansion of Weekend College, Doctor of Physical Therapy, Accelerated Bachelor of Science Degree in Nursing, Masters of Art in the Humanities degrees and an MBA program. Dr. Doud established 49 new endowed and expandable student scholarships totaling more than $19 million. Upon her retirement from the Mount, she was honored with the title of President Emerita by the Board of Trustees. A retirement gala in her honor raised more than half a million dollars for the newly created Robert E. Doud and Jacqueline Powers Doud Scholarship Fund.