Käroliis Toome has worked as a general practitioner at a health center in Finland, including positions in the health center's inpatient department and emergency room. She has also served as an assistant physician at the Pelgulinna Maternity Hospital, an assistant nurse and resident physician at Tallinn Children's Hospital, and as a general practitioner at Confido Medical Center. Käroliis Toome is a member of the Perinatology Society, the Estonian Young Doctors Association, and the Estonian Medical Association.