Gargamel

*NOTE: The sounds clips and editor's opinion were created by Pokejedservo. 

Hank Azaria - While I know that not a lot of people liked the live-action Smurfs movies (I personally did), in which Hank Azaria was a fine choice to inherit the role from the late, great Paul Winchell, he plays the role very closely to how the originator did (in both live-action and voice-acting).

Andre Sogliuzzo - Andre was pretty much hired to try and impersonate Hank's take on the role, but while his attempt isn't too bad, it clearly doesn't sound like Hank's voice, as it was way too rough and scratchy. (However, I do kind of like how Andre adds in a slightly more European accent to the role.) While I find Andre's voice rather forced at times, his performance overall was pretty solid and had a suitably "over-the-top" feel to it, which works pretty well. So, in other words, Andre's work on the role is pretty good on its own merits, but it's a rather so-so attempt at impersonating Hank Azaria. 

Overall, I am going with Paul and Hank the most, and Andre at a decent second place. 

-Pokejedservo