You can't beat a good super-villain ... unless your name is Bond.
1. Ernst Stavro Blofeld (Donald Pleasence, You Only Live Twice) - The head of SPECTRE had more opportunities than most to kill off Bond, having some involvement in six of the films. This must make him either the most resilient or the least successful of Bond adversaries. His first film appearances (From Russia With Love & Thunderball) kept his face and identity hidden, revealing only his hands and voice. This added an element of mystery to the character as the unseen controlling influence behind each villainous plot. However, it's Donald Pleasence's performance that brought Blofeld to life and confirmed his status as the greatest of Bond's opponents.
2. Auric Goldfinger (Gert Fröbe, Goldfinger) - With Bond strapped to a table and a massive laser about to slice him in two, 007 asks if Goldfinger expects this to make him to talk. Goldfingers response "No Mr Bond, I expect you to die!" is undoubtedly my favourite quote from any Bond film. The irony is that even in this seemingly helpless situation, Goldfinger still fails to finish Bond off. In the end it's Goldfinger that croaks, getting sucked out of a plane after shooting at Bond and cracking the window.
3. Dr. Julius No (Joseph Wiseman, Dr. No) - Initially comes across as an intelligent and ruthless foe, Dr No is eventually revealed to be a slightly unhinged psychotic nut. Despite several attempts to kill Bond off he never quite succeeds and is eventually killed by boiling to death in the coolant tank of his own nuclear reactor. In the novel he is killed by being buried under a massive heap of guano, the harvesting of which was supposed to provide a legitimate cover for his real activities.
4. Rosa Klebb (Lotte Lenya, From Russia with Love) - Quite possibly the scariest of all Bond's enemies, Klebb is Blofeld's leading agent in From Russia With Love, having formally been a member of SMERSH. In the final scenes of the film, at a point when it seems the action is over, she gains entry to Bond's apartment dressed as a maid to try and recover a cryptographic device. After a brief scuffle she makes an unsuccessful attempt on Bond's life, attempting to kill him with poison tipped spikes in her shoes.
5. Francisco Scaramanga (Christopher Lee, The Man with the Golden Gun) - Three nipples and a gold-plated single-shot pistol constructed from a pen, a lighter, some cuff links and a cigarette case. Scaramanga is a man very much in Bond's mold and proves a tricky foe to dispatch.