It's been a while since I read this one, but I do believe she gives up pursuing him after which he realises his feelings. And if I remember incorrectly, it's still a reaaaally good story:
https://www.mangago.zone/read-manga/untouchable_massstar/
The ML disliked the FL prior to reincarnation and initially didn't want to enter a relationship. But as she continues to draw a line between them in their contractual relationship, he realises how much he cares for her:
https://www.mangago.zone/read-manga/happy_ending_for_the_time_limited_villainess/
Prior to reincarnation the FL made the ML really uncomfortable in her persuit of him. First thing the "new FL" did was set him free and now he's the one pursuing her:
https://www.mangago.zone/read-manga/the_villainess_is_a_marionette/
Found this one today, actually. Also a reincarnation story with an obsessive villainess pursuing a man against his will, until another woman possesses her body and breaks it off:
https://www.mangago.zone/read-manga/the_tyrant_s_only_perfumer/
Oh, also this one:
https://www.mangago.zone/read-manga/i_want_to_do_it_even_if_it_hurts/
FL had an unrequited crush on a uni sunbae, who is anything but interested in love. So, when he needs someone to enter into a contract marriage for a short while, she volunteers. As their time together is coming to an end, he's realising his feelings for her.
yours to claim but it's a love triangle bestie so goodluck
Any romance manga (bl or straight) where in after the mc decided to stop pursuing the ml/leaves him (unrequited love), will the ml realize their love for her/him (mc).