But it was the harrowing scenes from a children's hospital in El Salvador which gave the actor his wake-up call.
He played the secret agent for 12 years, making him one of the most recognized actors around the world.
Moore told the BBC's Hardtalk: "I felt small, insignificant and rather ashamed that I had travelled so much making films and ignored what was going on around me."
He became a Unicef ambassador after My Fair Lady actress Audrey Hepburn introduced him to the charity's work 11 years ago.
He travelled to Central America and was struck with amazement when he watched as children saw running water from a tap for the first time.
But it was the harrowing scenes from a children's hospital in El Salvador which gave the actor his wake-up call.
"There was a child sitting without limbs, just rocking," he said.
"She had lost her limbs in a land mine that had killed her sister. Her parents were already dead.
"This poor limbless creature without any family was there on a hospital bed."
Moore now travels around the world fund-raising and campaigning to end cruelty to children.
The actor, whose career spans more than 50 years, is very grateful for playing a host of roles including 1960s TV hero The Saint.
For Moore, playing James Bond was also a life-changing experience.
But as a passionate opponent of the use of weapons, he is unhappy that his image with a gun is used throughout the world as a symbol of heroism.
He does recognise that playing the secret agent has brought him notoriety, which is useful for his work with Unicef.
Moore, who openly deplores the use of violence, brought his own tongue-in-cheek style to the James Bond films.
Sean Connery played a tougher Bond but Moore does not believe 007 would be quite so courageous.
'Long in the tooth'
"I don't believe in heroes because I know that I'm completely unheroic myself, a terrible coward.
"I tried to play it so the audience knows I'm having fun and I want them to have fun, it's not a private joke."
Moore made his Bond debut in Live and Let Die and bowed out in A View To A Kill in 1985.
"I was beginning to get a bit long in the tooth.
"If they are going to have a leading lady that matches up to you in age, she is already going to be a grandmother.
"That's not quite what James Bond is about."
HARDtalk with Roger Moore is on BBC News 24 on Wednesday at 2230GMT.