Sure. A bit hard to measure, but all the indicators are there. At least the Governor almost remade himself, even if he had a hard relapse, so that rules him out I think. Negan's always been shown to have humanity, if somewhat lacking.
Simon and Alpha are top-notch candidates for the title.
I still think the Governer was more evil. Alpha attacked the communities and set borders by marking one with heads, but she still seemed like she was only after her daughter in the end. Killing the group would just be a small bonus.
Simon is also up there but it seemed like he drew a boundry at killing his own men unless they turned on him. We didn't really see too much of him killing Saviors, just the Scavengers and Oceanside.
The Governer killed anyone who crossed him once Michonne killed his zombified daughter. He killed a fuck ton of Woodbury residents, anyone who could take leadership at the river camp, and the members of the prison. The Governer would not have stopped his rampage, and in the end, his ruthlessness was his downfall when he let his guard down while strangling Rick.
Honestly I consider the governor, Gareth, and Shane to be on the more lesser evil side of the villain spectrum. Cause I feel like they had a lot more sympathetic aspects to them. Not saying that their actions are completely justified or excused but you could at least understand to a degree where they were coming from and sympathize with them a little bit. Again not trying to justify or excuse their actions but still. They pretty much became villains due to the shitty world they lived in without anyone to keep them from keeping them (with the exception of Shane since he kinda had some anger problems once rick came back from the coma). Now with Alpha, she was already a shitty person and treated her husband and daughter like shit. And she only became more and more sadistic and evil as the years went by.
The Governor was barking mad, which actually helps his case a little bit (just a little bit). As much as I think Alpha's a crazy bitch with horribly, horribly stupid ambitions (if she wins, they go back to living in the cold woods, eating boar forever, and slowly dying of common ailments), she seems lucid. Oh, I'm sure a shrink could diagnose her with a thing or two, but those are her decisions, through and through.
Then we have the Governor who's screaming like a lunatic about how he doesn't "want it" while beating his former not-quite-friend with a golf club, like he's at open conflict with himself. He's a ticking time-bomb with no impulse control. So he's evil, but his redemption arc in Season 4 might have had more pay-off if he had access to some sort of prescription antipsychotic.
Going with Negan cause he was "the bad guy" for the longest time on the series.
As for the most evil probably Alpha.
But honestly no one here is really "evil". Every villian on the show seems to have been a normal person before the apocalypse and it was just the rnd of the world or their situation put them in their spot. But Alpha took it too far for the most part.
If I had to make a list of all the really evil villains in the series, I’d choose:
Alpha, Jocelyn, Beta, Dante, Simon, Jared (Savior), David (Savior), Gunther (Savior), Ed, the crazed man that the termites captured who was a rapist, Joe and the entirety of the claimers, Owen and the entirety of the wolves, Andrew (Prison), Tomas (Prison), Pete Andersen, Gorman, and Brandon