(Only movies dealing with post-WWII espionage are covered in this list.) 

The 60s run of "spy films" began with the first James Bond films, which set the tone by completely copping-out from dealing with the realities of espionage and the Cold War, opting instead for ridiculous "super-villains" and infantile "evil plots". Many subsequent 60s "spy" films treated espionage as even more of a joke, while a few others seemed to react against the unreality and stupidity of Bond, Flint, Helm, etc.    In the middle of this list are some 60s "nuclear crisis" and Cold War films that don't deal with espionage, but deal more closely with Cold War issues than most of the "spy" films. Like the "spy" films, but maybe to a lesser extent, they generally fall over themselves to remain apolitical.

After that, I list lesser known foreign (French, German, Italian, etc.) spy movies. 

Scores out of ten for the ones I've seen.

Tony Curtis, Janet Leigh, and Dean Martin in Who Was That Lady? (1960)

You Only Die Twice (EuroSpy Films & James Bond copies)

Jean-Paul Belmondo in The Professional (1981)

Sean Connery and Ursula Andress in Dr. No (1962)

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