Plenty.
Amrish Puri in Mr India. He is the soul of that film and prime reason why film is still memorable.
Amjad Khan as Gabbar Singh in Sholay was top notch villain and worth the chase, worthy of needing 2 men like Amitabh and Dharam fight against him.
Kajol in Gupt is the soul of that film. The film is nothing without her obsessive character.
Ashutosh Rana in Dushman and Sangharsh is the one who adds the spine chilling suspense in the films.
Ajit in Zanjeer and Kaalicharan is frankly more charismatic than the hero and a worthy challenge.
I also felt Kabir Bedi was a hugely charismatic and effective villain in Yalgaar and Khoon bhari maang.
Amrish IMO is generally top class in whatever films he does and shines even in less known or B grade films, both as character actor and villain.
Lalita Pawar is iconic as the bitchy saas or sauteli ma in most old films she did. So effective that it is her face that comes to mind when you think of evil MIL.
I believe solid villains, antagonists and well written character actors elevate a film and are a worthy challenge or support to hero and heroine.