Bayan rabuwar iyayenta a 1976, Jolie da dan uwanta sun zauna tare da mahaifiyarsu, wacce ta yi watsi da burinta na yin wasan kwaikwayo don mai da hankali kan renon 'ya'yanta. Mahaifiyarta ta tashe ta Katolika, amma ba ta buƙatar ta je coci. A matsayin yarinya, sau da yawa tana kallon fina-finai tare da mahaifiyarta kuma wannan ne, maimakon aikin mahaifinta mai nasara, wanda ya sa ta sha'awar yin wasan kwaikwayo, kodayake yana da shekaru biyar tana da wani ɓangare a Voight's Lookin 'to Get Out (1982). Lokacin da Jolie ke da shekaru shida, Bertrand da abokin zama, mai shirya fina-finai Bill Day, suka koma iyalin zuwa Palisades, New York; sun koma Los Angeles shekaru biyar bayan haka. Jolie sai ta yanke shawarar yin aiki kuma ta shiga Cibiyar Lee Strasberg Theatre, inda ta horar da shekaru biyu kuma ta bayyana a cikin shirye-shiryen wasan kwaikwayo Tambaya: Me Jolie ya yi a makaranta?
Cibiyar wasan kwaikwayo ta Lee Strasberg