Carmen Aldunate studied, from the age of 17, at the Escuela de Bellas Artes of the Universidad Católica de Chile, and subsequently joined the Facultad de Bellas Artes of the University of Chile. She was a student of Mario Carreno, Roser Bru, Nemesio Antunez, Delia del Carril, Mario Toral and José Balmes. Aldunate also spent a period of time studying at the University of California, Davis, where she made contact with Wayne Thiebaud and Willem de Kooning. Her first solo exhibition took place in 1963, and she held solo exhibitions in the USA and Peru during her early career. Her first retrospective exhibition, Diez años de pintura de Carmen Aldunate, took place at the Museo Nacional de Bellas Artes de Santiago in 1981. In 1997 the solo exhibition Pecados y Virtudes travelled to Valparaíso, Valdivia y Puerto Montt (Chile).
Aldunate taught painting and drawing at the Universidad Catolica de Chile, amongst other institutions, and has also produced illustrations for several important works of literature. She has participated in international group shows throughout her career, including the XII Bienal Internacional de São Paulo; amongst other awards, she received first prize (painting) at the 1962 Feria de artes plásticas de Santiago, first prize (drawing) at the 1974 Salón Oficial de Santiago, first prize (drawing) at the 1975 Bienal de Valparaíso, first prize at the 1978 Bienal de Punta del Este, Uruguay and first prize (drawing) at the 1981 Bienal de Cali, Colombia. In 2006 her work was included in an exhibition of Chilean artists entitled Arte Chileno Traspasando Fronteras travelling from Zagreb (Croatia) to Prague, (Czech Republic), Warsaw (Poland), Istanbul (Turkey) and Budapest (Hungary).