David Cameron was quick to pay tribute and described Frost as "an extraordinary man - with charm, wit, talent, intelligence and warmth in equal measure" who had "made a huge impact on television and politics".
"The Nixon interviews were among the great broadcast moments - but there were many other brilliant interviews," Cameron said.
"He could be - and certainly was with me - both a friend and a fearsome interviewer."
Actor and comedian Stephen Fry said he had spoken to Frost only on Friday and he had "sounded so well" and was "excited about a house move, full of plans".
Former prime minister Tony Blair referred to Frost as a "huge figure in broadcasting, a great professional and a good friend".
Frost's award-winning interview style was considered non-aggressive, affable and effusive, but he had a talent for extracting intriguing information and revealing reactions from his subjects.
His roster of interviewees included virtually every US president and British prime minister during his working life.
His big break came when he co-created and hosted satirical show That Was The Week Was in the early 1960s.
In more recent times, he had hosted Breakfast with Frost on Sunday mornings (1993-2005) and panel game show Through The Keyhole (1987-2008).
He was currently working for Al Jazeera English and had recently interviewed Chilean novelist Isabel Allende and F1 driver Lewis Hamilton.
- PA