Screen stars Julie Christie and Sir Laurence Olivier, murder mystery writer Agatha Christie and Yorkshire-born sculptor Henry Moore, as well as poet and author Vita Sackville-West 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 from 1960 to 1978, 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 in the early 1960s worked with The Sunday Times Magazine on documentary subjects from mental health to loneliness.
Other portraits gifted to the gallery feature actors John Hurt and Alan Bates, writers Kingsley Amis and Graham Greene, musicians Yehudi Menuhin and George Melly and artist Barbara Hepworth.
Snowdon: A Life In View, runs at the National Portrait Gallery, London, from this September to June 21 next year.