I think
Adam was the most sympathetic 'Big Bad' because he was made of various parts, very much a product of his environment; he had a lot of the same traits as Frankenstein's monster, which I find tragic. He deserved better writing, to be honest. Season 4 writers seemed at a loss with how to handle him as well as the Initiative.
The best written 'Big Bad' was probably
Angelus, simply because of how much devastation he was able to cause in such a short space of time. His brutality reshaped the lives of the Scoobies, and his murder of Jenny still makes me rage.
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