The most famous of his novels, Tinker, Tailor, Soldier, Spy, follows ageing spymaster George Smiley as he hunts for a mole in The Circus, the author's fictional spy HQ.
But in contrast to the glamorous Bond novels of Ian Fleming, Le Carre's books portray the intelligence services as corrupt organisations filled with traitors, Dearlove said.
"We've all enjoyed enormously reading the Smiley books ... and he does capture some of the essence of what it was like in the Cold War.
"However, he is so corrosive in his view of MI6 that most professional SIS [Secret Intelligence Service] officers are pretty angry with him.
"Intelligence organisations are based on trust between colleagues. That's how they operate.
"His books are exclusively about betrayal. He writes in the tradition of the counter-intelligence nihilists."
Dearlove was "C", the head of MI6, between 1999 and 2004, and oversaw the intelligence agency's response to 9/11 and the invasion of Iraq.
He said Le Carre had become "obsessed" with his career as a spy, which began in the 1950s after he passed information to MI5 about left-wing groups at Oxford University.
"He was only in the service for three years, and something must have happened to him while he was there to breed this cynicism.
"I rather resent the fact that he is trading on his knowledge and his reputation, and yet the feeling I get is that he intensely dislikes the service and what it represents."
After leaving Oxford and teaching at Eton, Le Carre worked undercover in West Germany, running agents in the war of information against the Soviet Union. He waited more than 30 years before revealing his MI6 career, believing he'd endanger agents he had known in the 1960s.
His cover was blown by infamous double agent and Cambridge spy ring member Kim Philby.
Since then, the author says, his former colleagues have been furious with him for portraying them as "heartless incompetents" when they cannot answer back in public.
Former Labour Defence Secretary Denis Healey once called him a "communist spy" at a drinks party, and high-ranking officers believe he has profited from an exaggerated account of the MI6 in the Cold War.
Dearlove said Le Carre was not the only former spy to have written books about life in espionage, but he was one of the key "mythmakers".
New MI6 officers now have to sign over the copyright to any future books before they join the service, to prevent them making money out of the job.
Le Carre's men
• "Smiley was the oddest. You thought, to look at him, that he couldn't cross the road alone, but you might as well have offered protection to a hedgehog."
Tinker, Tailor, Soldier, Spy
• "He met failure as one day he would probably meet death, with cynical resentment and the courage of a solitary."
The Spy Who Came in From the Cold
• "He appeared to spend a lot of money on really bad clothes, which hung about his squat frame like skin on a shrunken toad."
Call for the Dead
• "A professional intelligence officer is no more immune to human feelings than the rest of mankind. What matters is the extent to which he is able to suppress them."
A Legacy of Spies
• "He had grown a trivial moustache, like a scrawl on a photograph, which made a muddle of his face without concealing his shortcomings."
The Looking Glass War
