The former James Bond star jokingly suggested Craig had such an air of menace in his performance as the character that he felt he was capable of being a killer.
Speaking to an audience at the Southbank Centre, London, the veteran actor did not rule out a cameo role in a future 007 film to “expand the family coffers”, but denied having received any offers.
Sir Roger is the longest-serving actor to play the womanising MI6 agent, having portrayed him for seven films.
Asked by an audience member who he felt was the best Bond, he told the packed auditorium: “I think that Sean was obviously the great Bond.
“He was obviously the right person, he brought the right personality to the performance, otherwise Bond would not have gone on past the first six that he did. He was a tremendous Bond.
“Today, I think we’re very lucky to have Daniel Craig because he is quite extraordinary, I always say that Sean looked like a killer - but Daniel Craig would finish it off.
“When I saw Casino Royale, I thought that Daniel Craig did more action in the first seven minutes than I did in seven movies.”
The 89-year-old began the talk by defiantly marching on the stage holding a large plastic poppy - a protest, he said, against Fifa’s decision to ban players from having the commemorative symbol on their shirts.
Then, taking a seat on a chair boasting a cushion with the British flag on it, he announced: “Nicola Sturgeon, eat your heart out.”
During the 90-minute talk, Sir Roger went through his career and his time working alongside some of cinema’s most accomplished performers.
But, despite landing perhaps the most coveted role in the film industry, he said there was another leading character he wished he could have played - Lawrence of Arabia.
“I remember Bob Baker and I going to see Lawrence of Arabia and coming out both being very depressed and saying ‘we might as well give up the business’, because they had made the best movie that had ever been made,” he said.
The event was hosted as part of the Being a Man festival at the venue, which was launched to “celebrate and interrogate masculinity in all its variety and hidden depths”.