I like the list. Lee Van Cleef takes it in many ways because his role was essentially always the villain.
They list Lee Marvin as Liberty Valance; good enough, but he was a bit over the top there. He was even smoother as the wicked guy in Seven Men From Now with Randolph Scott, a classic performance. Likewise, Richard Boone was a great bad guy as Cicero Grimes in Hombre, but almost as good in The Tall T; that one also with Randolph Scott.
But though both Marvin and Boone made great villains, they had too many other non-villainous roles to be pigeonholed as great villains.