Although the moves were made in response to a call from the Vatican to modernize, conservative Cardinal James Francis McIntyre of the Los Angeles Archdiocese barred the sisters from teaching in the Catholic schools he oversaw.
As of last year, it remained the largest Catholic order in the U.S. to sever ties with the Vatican, according to the 2010 edition of "Unveiled: The Hidden Lives of Nuns."
The ex-nuns came together to found the Immaculate Heart Community, an independent ecumenical organization that marked its 40th anniversary last year. It has 160 members today.
Caspary, who served as the order's final leader and the community's first president, died Oct. 5 at the group's retirement home in Los Angeles, said Lenore Dowling, an organization spokeswoman. A cause of death was not released. Caspary was 95.
"While I saw the break as inevitable, I didn't really want it," Caspary said in 1970 in Time magazine, which featured her and a former bishop on the cover below the headline "The Catholic Exodus: Why Priests and Nuns Are Quitting."
"But I wondered how much energy you could spend fighting authority when you could spend that same energy doing what you should be doing," Caspary told the magazine.
Many community members continued careers in education while others pursued law, social work, inner-city development or other endeavors. Caspary served as its president until 1973.
"She had intellectual strength," said Susan Maloney, a scholar on women in religion who cared for Caspary in recent years. "Her leadership, her personality style had a demeanor that was inviting and challenging."
Anita Marie Caspary was born in 1915 in Herrick, S.D., the third of eight children of Jacob and Marie Caspary. Two of her siblings died very young.
She grew up in Los Angeles in an actively Catholic family and attended Immaculate Heart College, founded by the sisters. As she worked toward her bachelor's degree in English, Caspary developed an appreciation for the independent-minded nuns.
"Even then they weren't all in lock step," she told Time in 1970.
After graduating in 1936, she entered the convent and began teaching English at Immaculate Heart High School, established by the order in 1906 in Los Feliz.
She earned a master's degree in English at USC in the early 1940s and a doctorate in English literature at Stanford University in 1948.
While wearing her nun's habit at Stanford, she felt it created both "a distance and mystery," she wrote in her memoir.
Upon returning to Immaculate Heart College, she chaired the English department and was the graduate dean for much of the 1950s. In 1958, she became president of the college and served until 1963, when she was elected to lead the Immaculate Heart order.
The order's most famous alumna, Corita Kent — the artist best known for the "Love" stamp — said of Caspary in 1970 in Time: "She is a quiet leader, perfect for the age of Aquarius, when, you know, there are no big heads."
As the order relaxed the strict rules that governed convent life, sisters were allowed to use their given names. She dropped her religious name, Sister Humiliata.
In the 1970s, she taught at the Franciscan School of Theology and the Graduate Theological Union in Berkeley.
Returning to Los Angeles, she worked with the Peace and Justice Center of Southern California in the 1980s and also taught courses on feminist spirituality at the Immaculate Heart College Center, established after Immaculate Heart College closed in 1980.
At 85, Caspary secured a grant to teach poetry to older women who lived in her retirement home.
Decades after the order's dramatic struggle, she saw it in historical terms, writing in her memoir: "In many ways, we foreshadowed the contemporary (and vibrant) feminist movement within the Catholic Church."
Caspary is survived by three sisters, Gretchen De Stefano of Los Alamitos, Marion Roxstrom of Newport Beach and Ursula Caspary Frankel of Costa Mesa; and a brother, Gerard Caspary of Las Vegas.
A funeral Mass will be celebrated at 9 a.m. Saturday at Immaculate Heart High School, 5515 Franklin Ave., Los Angeles.