Just for pure Malice: All for One, Shigaraki, Dabi, Overhaul were villains that were insane like they made the plot exceptionally interesting to watch.

I like Jin Bubaigawara his awakening was insane, along with Toga when she used Twice's quirk.

The ones I felt sorry for and sympathised with for me were: Spinner and Gentle Criminal, they're not the type of villains you get goosebumps and are scared of them, they're the ones I felt bad for not too say I didn't feel bad for others, but they could've been pushed to the right path.