Like most young women of her class, Wald led an active social life, but at the age of sixteen she decided that she needed more serious work. She applied to Vassar College, but was refused due to her youth. Soon thereafter, Lillian attended the birth of her sister Julia's child. She was so inspired by the work of the attending nurse that she decided to embark on a career in nursing.

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In 1889, Wald enrolled in the nursing program at the New York Hospital Training School. After her graduation in 1891, she went to work as a professional nurse at the New York Juvenile Asylum, an orphanage for children ages five to fourteen, but she quickly became disillusioned with institutional methods of caring for children. As Wald's earliest biographer, journalist and friend R. L. Duffus, wrote, "she had too much individuality to be willing to lose herself as a cog in an established institution. Instinctively, she wanted to change things—to do better." In 1892, she enrolled at the Women's Medical College in NYC.