Jeffrey was home schooled and went on to received her Bachelor from the University of London in 1919. Since her family couldn"t afford to support her through doctoral training, she instead got a teaching diploma in 1920. Later on, she was able to return to school and received her postgraduate diploma in individual psychology in 1945.
Jeffrey began her career as a music and English teacher. Once she received her postgraduate diploma in individual psychology, she began working in the field of child guidance. She and a colleague both noticed that the rules set for staff got in the way of effective therapy, so her colleague founded the Open Way Association and Jeffrey joined as a psychotherapist.
Later on, Jeffrey opened up a private practice.
Carol Jeffrey published a semiautobiography towards the end of her life called That Why Child. This book discussed her perception of the causes of child psychopathology.
