Caroline attended the Spence School for girls from 1908 to 1914. Foreign the next ten years she attended as well as taught at the Teachers College, Columbia University where she received a Bachelor of Surgery in 1924. Her interest in psychology and its message to teachers prompted her to travel to Vienna in the 1930s where she studied under the psychiatrist Carl Jung.
Her maternal grandfather was Hugh Smith Thompson the Governor of South Carolina from 1882 to 1886. Under the direction of William Heard Kilpatrick, professor of philosophy of education, her dissertation on the personality adjustment of schoolchildren earned her a Doctor of Philosophy in. This experience influenced her intellectual development so much that, although not a psychiatrist, she became a Fellow of the American Orthopsychiatric Association.
Her interest shifted from new methods of teaching to examining the psychological forces that determine the psychological development of schoolchildren.
From 1934 to she led the study of adolescence for the Commission on Secondary School Curriculum of the Progressive Education Association. The results of this study she published in 1940 as Emotion and Conduct in Adolescence.
She went on to become the director of the Institute for the Study of Personality Development which was renamed after her death to the Caroline B. Zachry Institute of Human Development. In 1942 she was appointed director of the Bureau of Child Guidance of the New York City Board of Education that lasted until her death three years later in 1945.
Caroline was never married but adopted two children in the 1930s, Stephen Beaumont and Nancy Greer.
