Born to the family of a coal miner, his acting talent was discovered very early and he won a scholarship with respected director Bojan Stupica. Samardžić was educated at the Belgrade Drama Arts Academy. After graduation, he obtained a role in Igre na skelama (1961).
Samardžić was a member of the Central Committee of Yugoslav Communist Party in late 1980s.
In the 1960s, he established himself as one of the most recognisable and popular stars of former Yugoslav cinema.
In the 1990s, he and his son Dragan Samardžić founded a film production company. Despite break-up of Yugoslavia and UN sanctions against Serbia, the company made many popular and commercial successful films.
In August 1995, he received Life Achievement Award "Pavle Vujisić" for his roles in Yugoslav cinematography.
He has been married to Mirjana Samardžić since 1960. Nicknamed Smoki, he has been credited as Ljubisa Samardjic, Luba Samardy, Ljubisa Samardzic-Smoki, and Smoki Samardì.
- The Climber (1966)
- Battle of Neretva (1969)
- In Love, Every Pleasure Has Its Pain (1971)
- The Tiger (1978)
- Premeditated Murder (1995)
- Yu (2003)