Although I think they both are really good villains in their own way but if I had pick one I'm going with Yosemite Sam.

Ok.

But, I'm going with more Polite, Sophisticated, Affable, Calculating, Tech-Smart, Science-Fiction and Intelligent type of Villains, Thank you very much.

So, NectariaKiritsi, What is your opinion of Yosemite Sam, and What is your opinion of Marvin The Martian?, I find Yosemite Sam is Rude, Loud, Trigger-Happy, Short-Tempered, Hot-Headed, Aggressive and Constantly Foul-Mouthed in Gibberish. But Marvin The Martian on the other hand is more Calm, Soft-Spoken, Refined, Sophisticated, Intelligent, Affable, Gentlemanly and Polite. Unlike Yosemite Sam, who is angry in the aggressive and hot-headed way, Marvin The Martian is angry in the calm, tranquil and gentlemanly way.