The first three with Sean Connery or any with Daniel Craig. The ones in between were blah although the women were beautiful, and Roger Moore made Bond into a comic book character.
Fleming's original Bond was an assassin and a borderline alcoholic, he smoked and drank way too much. He knew some fancy fighting moves but used mostly what would have been taught to British Commandos in the war, not a lot of hai karate stuff. Later in his career the people he killed started to weigh on his conscience.
Craig, despite his political views, brings a lot more edge back into the role.