Top 3 Roles?

Champagne for Caesar - which demonstrates a wonderful gift for comedy that was infrequently tapped. He is hilarious, a joy.
Witchfinder General
The Masque of the Red Death

Bump

laura
The Masque of the Red Death
House of Usher

Let's not forget...Egghead, in the Batman series.

Otherwise, just about anything else:
Pit and the Pendulum
House of Usher
Edward Scissorhands

I used to live for the opportunity to see the old films on broadcast TV - when antennas were the delivery mechanism.

His Kind of Woman
The Baron of Arizona
The Abominable Dr. Phibes

(some excellent, non-hammy, non-horror acting by Vincent Price):
The Ringmaster | Robert Montgomery Presents (1952)
https://youtu.be/vP6EVVhrc_Y