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Mother Margaret Mary Brady held several administrative positions in the Sisters of St. Joseph community before 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 fall. Despite sparse finances and the Great Depression, she oversaw the successful construction of the first building at Chalon, now called Brady Hall, which was occupied in 1930. She also launched the 12-year fund raising effort for the future Mary Chapel. Today, the annual Brady Award is given to a student who entered Mount Saint Mary's beyond the age of traditional college undergraduate students.

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, Mannix 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. After completing her six-year term in 1943, she continued to teach until 1958.

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 teaching credentials. The draw of these prestigious programs and a growing student population required new construction. Overcoming wartime rationing in building materials, the Mount built St. Joseph Hall in 1944 with new science labs, classrooms, a theater and administrative offices. That same year, Le May purchased an additional 21.7 acres of land, increasing the Chalon Campus to nearly its present size. In 1946, the Charles Willard Coe Memorial Library was built with funds left to Sister Mary Celine Coe, CSJ, by her rancher father. Le May launched The View, the campus newspaper, as well as the Mount yearbook and Alumnae Echoes newsletter.

Mother Agnes Marie O'Loughlin, the Mount's fourth 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, the first baccalaureate nursing program in California, was launched in 1948. In 1953, the Mount joined 10 other colleges to form the Independent Colleges of Southern California (ICSC).

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.

A 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 before becoming the Mount’s sixth president. 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. Calloway negotiated with Cardinal McIntyre to assume ownership of several of its Victorian mansions for the CSJs and the college. Like her predecessors, Calloway 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 Saint Mary’s University, she planned to launch a two-year associate in arts degree program in September 1962 on the new downtown campus, making the Mount the first Catholic college on the West Coast to offer an AA degree. But before she could give her full attention to the new program, the Bel Air fire destroyed one-fifth of the Chalon Campus and part of Carondelet Center in November 1961. Early the following year, she announced a $10-million long-range development plan to raise money to expand both campuses. In 1965, the Humanities Building added much-needed classroom space at Chalon, and a new classroom building and auditorium became the first new construction at Chester Place since the early 20th century.

As Sister Cecilia Louise Moore began her presidency, Mount Saint Mary’s University was starting to reflect some of the significant changes occurring in society, higher education and the post-Vatican II Church. 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, Moore negotiated with Cardinals McIntyre and Manning for title to the remaining Doheny property, giving the Mount both sides of Chester Place and a strong foundation for the future.

The Mount began its second 50 years with Sister Magdalen Coughlin as president. Seeing education as an investment in the future leadership of California and the nation, Coughlin 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 Saint Mary’s University, 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 new library named for Mount supporter J. Thomas McCarthy. The Mount's outreach to nontraditional students took on its current form in 1992 with the establishment of what is now Weekend/Evening & Online College, and the nursing programs were expanded to meet the growing demand for healthcare professionals.

Jacqueline Powers Doud, the 11th president of Mount Saint Mary’s University, served °ÄÃŲʿª½±ÀúÊ·½á¹û as provost and vice president for academic affairs before becoming the College's first lay president on July 1, 2000. She had more than 30 years of experience in senior administration, serving the University of La Verne, Woodbury University and Mount Saint Mary's, after 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 Doud's tenure included an expansion of Weekend/Evening & Online College and new degrees, including a Doctor of Physical Therapy, Accelerated Bachelor of Science Degree in Nursing, Master of Art in humanities and an MBA. 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.