Frank Gorshin was the best Riddler. It was his idea for the character to wear a suit at times, and he did just a fine job of playing the role and making it his own. He also had a better, creepier laugh than the Joker.
John Astin wasn't as good for the role but he played out Riddler's narcissism well.
John Glover was a great Riddler. The BTAS creators changed up Riddler (to make him more unique in comparison to Joker) and Glover really seemed to know what they wanted; a colder Riddler prone to mood swings but who is often quite reserved and not so manic.
Robert Englund played a more gothic version of Riddler, and I think he did a very good job of making the character sound more sinister.
There's also Ted Knight (Batman/Superman Hour), Michael Bell (Challenge of the Superfriends), John Michael Higgins (Batman Brave & The Bold), and Dave Franco (Young Justice) who were all pretty good. Ted Knight made Riddler sound as annoying as possible (which makes sense). Michael Bell, Higgins, and Franco had a similar approach, just not as annoying.
Wally Wingert (Arkham Asylum, Arkham City) is another great Riddler voice actor, kind of manages to mix up the styles of Gorshin, Glover, and Jim Carrey into his own. I thought the voice effect given to Riddler in AC was pretty interesting too, making him even more of a psycho troll to Batman.
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