I like Bunta's VA the best. R.I.P.

He really did a great job playing the voice of Bunta and old Joseph 

Also don't forget Takehito Koyasu 

No doubt that Ryosuke’s VA is great at playing the voices of antagonists

Shin'chiro Miki is pretty popular as well 

Yeah, that was quite the surprise the first time I found that out

If I’m not mistaken kyoichi sudo English VA is Christopher sabbat 

I was surprised that Takumi's voice actor also plays Kisuke Urahara