Premnath dated the famous actress Madhubala but ended it when she became interested in actor Dilip Kumar.

In 1951, Nath starred opposite Madhubala in Badal which was a big box office success.

He went on to appear in many films in leading roles often opposite his wife Bina Rai which failed to do well.

He started receiving recognition with playing the central villain or supporting role in some of the biggest blockbusters in Indian film history throughout the 1970s.

Some of his notable films included Teesri Manzil (1966), Johny Mera Naam (1970), Tere Mere Sapne (1971), Shor (1972), Bobby (1973), Roti Kapda Aur Makaan (1974), Dharmatma (1975), Kalicharan (1976), Krodhi (1981) and Desh Premee (1982).

He earned Filmfare nominations as Best Supporting Actor for: Shor (1972), Bobby (1973), Amir Garib (1974) and Roti Kapda Aur Makaan (1974).