Randriambololona was born in Anjozorobe, Madagascar and was ordained to the priesthood in 1961 for the Society of Jesus. He served as coadjutor bishop of the Roman Catholic Diocese of Antsirabé, Madagascar, from 1988 to 1989 and then as bishop of the diocese from 1989 to 1992. He then served as the archbishop of the Roman Catholic Archdiocese of Fianarantsoa, Madagascar from 1992 to 2002.