Angelito Castro Anzures was born to Felix Anzures and Juliana Castro in 1927. He studied at the Marcelo H. del Pilar Elementary School and finished his secondary education at Bulacan Academy, Bulacan. Using his nickname "Lito" for films, he first appeared in Halik Sa Bandila (1948), followed by Sigaw ng Digmaan (1963), Tanging Ikaw (1968), Sorrento (1968), Romantika (1970), Mga Anghel na Walang Langit (1970), Ang Kampana ng Santa Quiteria (1971), Daluyong at Habagat (1976) and Ibilanggo Si Nene Magtanggol (1977). Goodlooking and dramatic, he appeared in 7 films opposite movie star Fernando Poe Jr., including Sigaw ng Digmaan, Tanging Ikaw, Sorrento, Ang Pagbabalik ni Daniel Barron (1968), Asedillo (1971), Agila ng Maynila (1989) and Wanted: Pamilya Banal (1989). In 1963, he received a best supporting actor award from the Film Academy of Movie Arts & Sciences (FAMAS) for his performance in Sigaw ng Digmaan; ironically, his first starring role, not supporting. In 1985 he received best supporting actor citations from Star Awards and Manunuri ng Pelikulang Pilipino (MANUNURI) for Paradise Inn (1985). After a slew of supporting actor nominations and awards, he was finally nominated as Best Actor for Ang Pinakamandang Hayop sa Balat ng Lupa (1974) by FAMAS.