Screen stars Julie Christie and Sir Laurence Olivier, murder mystery writer Agatha Christie and artist Henry Moore are among the figures featured.
The donation of 130 photographs from Lord Snowdon's archive is one of the largest gifts ever received by the gallery and several of the portraits will go on display for the first time this autumn.
Lord Snowdon, who was married to Princess Margaret, turned his lens on the worlds of theatre, fashion and high society when he began his career in the 1950s.
He is known for his six-decade association with Vogue and he also worked with the Sunday Times Magazine on subjects from mental health to loneliness.
The gallery's director, Sandy Nairne, said: "The National Portrait Gallery is delighted that Lord Snowdon should have made such a generous further gift of prints to the collection.
"These are wonderful portrait images of some most creative and engaging contributors to Britain in the second half of the 20th century."
Snowdon: A Life In View, runs at the National Portrait Gallery, London, from September 26 to June 21, 2015.