Angelita received scant school instruction, as was usual at that time among girls in her social class; by the age of 12 she went to work in a shoe-making workshop to contribute to the family income. She was employed there with brief periods of interruption until the age of 29, under the fortunate care of a highly devout businesswoman who encouraged Angelita and the other workers to pray the rosary together and to read the lives of the Saints.
At the age of 19, Angelita requested entry into a convent of Discalced Carmelites but was not admitted due to her weak health; four years later she tried religious life again by joining the Daughters of Charity of St. Vincent de Paul in which, during her novitiate, she was sent first to serve in a local hospital, and later in Cuenca and Valencia. At this time, however, the young woman's health unexpectedly declined and she was plagued with chronic vomiting, which eventually forced her to leave the Vincentians. Curiously, after her departure, the vomiting ceased as mysteriously as it had started, leaving no lasting effects. She returned to her former job in the shoe shop.
Sometime in 1873, Angelita had a decisive mystical vision in which she saw an empty cross in front of another cross on which Jesus was crucified. She instinctively understood that Christ was inviting her to sacrifice herself on the empty cross - to be "poor with the poor in order to bring them to Christ", per her own words - and she pronounced private vows of perpetual consecration to God. She also conceived the idea of founding a new charitable ministry, which she referred to as the "Company of the Cross".