Back in the beginning, I'd have to say that Goldfinger and Blofeld were among the best Bond villains because of the people that surrounded them. Blofeld had Rosa Klebb, Mr Wint and Mr Kidd (the lovers).
Goldfinger was great because he had Oddjob (who can forget the man with the killer hat), and Pussy Galore (who can forget that name).
In the 1980s, Max Zorin with May Day were an excellent duo. I love Christopher Walken.
Today would be Alec Trevelyan with Xenia Onatopp. You got to love a sociopath with a grudge and who hangs around with a freak who gets orgasms by killing men with her thighs. Come to think of it, that's the way I'd like to go.