No I believe you did the right thing. He needs to learn that he needs to quit overstepping boundries, and once they keep continuing, just break ties with them all together.
Believe me, I had a friend once who overstepped my boundaries even though I told them to stop.
The best thing is to break all contact with them.
And honestly Imgflip needs to step up their blocking privileges. Like the blocker should not be able to see your comments.