Silvertoe didn't? I know ironpony does though!
Carver for me. He, along with Klebb and Zorin fight it out to claim the 'Best Bond Villain' title from me. His showmanship persona and charisma combined with Feirstein's juicy monologues and fascinating characterisation allow for a very compelling villain. Pryce never seems to ham it up though, and strikes a great balance of theatricality (in itself a good contrast to Bond) and vulnerability. I mentioned recently when I rewatched TND how Spottiswoode manages to find some beautiful character moments and reactions even amid the chaos unfolding around them and that extends to Carver. His brooding on the stealth ship and after the party especially, when he sits alone reflecting on the decision he's just made to have his wife killed. And that rather engrossing scene where he confronts Paris about Bond's involvement in sabotaging his broadcast. He's truly an underrated villain and Pryce, as you suggest, is more than up to the task.
Elektra would round out my top 5 villains but she is arguably my favourite Bond girl. There's so much to love about her character but as I've said before: if I'm watching the film and I'm hoping she doesn't turn out to be the villain as suspected, Marceau and the film makers have achieved something extraordinary. I dig Trevelyan too. Pitting Bond up against a defected 00 is an inspired idea and adds so much to GoldenEye's discourse as well as its dramatic potential. His reveal and fight scene with Bond are particular highlights.
Graves is simply to hammy. A caricature of a villain. DAD would have played out better had we stuck with Col. Moon. Shame because Toby Stephens is a great actor. Perhaps he was just too young at the time.
Villains:
1. Elliot Carver
2. Elektra King
3. Alec Trevelyan
4. Gustav Graves
Henchmen
1. Xenia Onatopp (one of the classics!)
2. General Ouromov (Gottfried John is brilliant. Such screen presence.)
3. Dr. Kaufman (a chilling yet humorous cameo who draws out Brosnan's dark side)
4. Renard (a fascinating disability that somehow humanises a terrorist. The remember pleasure scene is a highlight).
5. Stamper (underrated Red Grant descendant. Some great one liners and physical presence).
6. Boris (Hilarious!)
7. Davidov (His desperate vulnerability is enough to make him stand out on his own).
8. Henry Gupta (Suitably slimy but can be overlooked due to the strength of TND's other villains.)
9. Zao (Should be more dangerous than he is but has a striking look.)