Love this trope too! Here's two recs for a good villain (actual villains, not anti-heroes) obsessive love story:
Obsessive villain dramas:
Khaani -This is a Pakistani drama I watched on Netflix recently. Only the villain is actually the male lead, so he's the hero as well. But I saw him as the villain because he's pretty much the main antagonist of the series and never gets the h's love.
I was only interested in the first 21 episodes (31 episodes in total) as that was all about how he came to be obsessed (wasn't right away and it was awesome watching the "falling" process) and stalked/chased after the h like an unyielding, bulldozing tank. Seriously, once the villain realizes his feelings, he's batsh*t crazy obsessed and nothing can deter him from trying to make the h his. He does many crazy things: Stalks her everyday, injured himself with a glass bottle so he can be a patient at the hospital where she works, threatened to kill himself when he found out his disapproving parents tried to kill the h (would have gone through with it if the h died for real), and forcing her to get engaged with him.
Seriously, the villain's one of the most obsessed I've ever seen and it doesn't hurt that he's absolutely gorgeous and shares explosive chemistry with the h. All their scenes together are gold and I just couldn't get enough of the way he looks at her like he wants to devour her. The villain's actor is very skilled and I loved all of his facial expressions (his eyes really exude emotion), esp. when he's around the h. He seriously can't bear to be away from the h once he falls for her. It's been a long time since I've felt this way about a pairing.
Sadly, this drama is a tragedy and the villain ends up serving a life sentence due to him murdering the h's brother. The h also married someone else (didn't bother me because she never loved the villain). I also didn't watch the last 10 episodes or so, because they strayed away from the romance and focused on the villain's redemption/seeking forgiveness for his past indiscretions. But the first 21 episodes is a must watch for anyone in the mood for a highly compelling "villain obsessively in love" storyline with hot hot chemistry btw the leads.
The drama's also got an amazing soundtrack.
Here are two mvs: One featuring the twisted romance and the other is the official ost mv::
https://www.youtube.com/watch?v=7kk2xXIJvlQ
https://www.youtube.com/watch?v=N1Erx5Vbh5U
Memory Lost -The villain's backstory and motivations were so compelling that my heart was absolutely shattered in the end. He really took obsession to the next level (erases the heroine's memories so he can start over with her) and I can't say he loved the heroine any less than the hero -she really was his entire world! He could give up anything and anyone in order to be with her. Even the other woman said it, "I knew an old friend who could turn against the whole world in order to possess the one thing he wants..."