There could be a group within the Fairy King's court that is against his cooperation with the wizarding world. They see humans as inferior and want to isolate the fairy realm again. They start causing trouble for Harry and his allies in the wizarding world, and they become the main antagonists as they try to undermine the relationship between the two worlds.
It could be a dark fairy who is jealous of the Fairy King's alliance with the wizarding world. This dark fairy wants to destroy the connection and take over both the fairy realm and the wizarding world.
A group of rogue Death Eaters could be the main antagonists. They think that Voldemort has gone soft by teaming up with Harry. So they break away and form their own more extreme and violent group. They start attacking both the wizarding world and anyone associated with Harry and Voldemort's new alliance. Harry and Voldemort must then fight against their former allies who have become a greater threat than ever.
It could be a rogue Death Eater who decides to carry on Voldemort's legacy in a more extreme way. This Death Eater might have some new and terrifying dark magic up their sleeve.
It could be a rogue Death Eater who wants to take over Voldemort's position and sees Harry and Bellatrix's new - found alliance as a threat. For example, a Death Eater who was always jealous of Bellatrix's closeness to Voldemort.
Maybe it's a rogue group of wizards who fear Harry's power over Dementors. They might think that Harry is going to use the Dementors to take over the wizarding world in an unjust way. So they band together to try and stop Harry before he can fully embrace his role as the King of Dementors.
It could be a powerful dark wizard who wants to control the spiders for his own evil purposes. He might see Harry as a threat to his plans since Harry is the 'King of the Spiders'. This wizard could be using dark spells to manipulate the spiders and turn them against Harry and the wizarding world.
The main antagonist could be Dumbledore. Since Harry has joined Voldemort, Dumbledore would see Harry as a threat to the good of the wizarding world. Dumbledore would try to bring Harry back to the right side, and they would end up in conflict.
It could be a follower of the God of Death who misinterprets the God's will and tries to bring chaos to the wizarding world. They might see Harry as an obstacle to their plans and try to eliminate him.
Another option could be a corrupted version of Merlin. What if he was turned evil by some dark magic? He would know all the secrets of both the Arthurian and wizarding worlds. He could use this knowledge to create chaos and try to rule over both. Harry and the good knights of Arthur would have to find a way to reverse his corruption.
In this fanfiction, it could be a group of corrupted magical nobles who oppose Harry's rule. They are used to having all the power in the alternate universe and don't want to give it up to an outsider like Harry. They could be plotting all sorts of schemes to undermine Harry, from spreading false rumors to outright attacking him and his supporters.
Perhaps a new dark wizard or witch who sees Harry as a threat. Since Harry has the power of Voldemort version 2, this new antagonist might fear that Harry will stop their plans for world domination. They could be someone who was in the shadows during Voldemort's time and now wants to take advantage of the chaos that Harry's transformation brings. They would try to use Harry's new identity against him and turn the wizarding world against him even more.