A possible main antagonist could be Aizen from 'Bleach' who somehow gains the ability to control the powers from Lucy's world as well. He could use this newfound power to try and take over both the Bleach universe and Lucy's world. His cunning and powerful abilities would make him a formidable foe for Lucy and the Bleach characters to face.
Maybe a new character that is a combination of the dark forces from both universes. This character could be a powerful wizard in Lucy's world who was corrupted by Hollow energy from 'Bleach'. He wants to merge the two worlds into a chaotic realm where he can rule supreme. So, he starts creating havoc in both worlds, which forces Lucy and the Bleach heroes to join forces against him.
The main antagonist could be a powerful and ancient fairy who has been banished long ago but now returns to seek revenge on the fairy world. And Lucy, being a new and important part of the fairy world, becomes a target. This antagonist might have unique and dark magic that makes it extremely difficult for Lucy to defeat. Also, the antagonist could have some sort of grudge against the fairy queen or king, and Lucy is caught in the middle of this power struggle.
Maybe some sort of combined form of Orochimaru and a powerful Hollow. Orochimaru is always after power and knowledge, and in this fanfiction, he could have somehow made his way into the Bleach world during Naruto's exile. The combined entity would be extremely dangerous, having both Orochimaru's cunning and the Hollow's brute strength.
Well, a cool plot might involve a Hollow in 'Bleach' escaping to the world where Lucy exists. Lucy, being the curious and strong - willed character she is, decides to track it down. Along the way, she meets some Soul Reapers who have also come to deal with the Hollow. They realize that Lucy has a special connection to the spiritual energy that could be used to defeat the Hollow more effectively. So, they join forces, with Lucy learning some Soul Reaper techniques and them learning about her world's magic.
A time - traveling bounty hunter could be the main antagonist. He might be after Lucy because she has somehow disrupted the time - space continuum. He's cold - hearted and will stop at nothing to bring her to some time - traveling justice.
It could be a dark wizard who wants to use the baby's power for his own evil deeds. Maybe the baby has some special magic that the wizard thinks can help him take over the magical world.
It could be another powerful celestial dragon who opposes Lucy's ideas or presence.
If it's a crossover with Alice in Wonderland, the Queen of Hearts could be the main antagonist. The Queen might see Tinkerbell as an intruder and try to behead her. Tinkerbell would have to use her wits and magic to survive in the crazy world ruled by the Queen of Hearts.
Aizen could be a great main antagonist. He's extremely intelligent and powerful in the Bleach universe. He might see the Miraculous as a means to further his own goals, whether it's to gain more power or to create more chaos. His manipulative nature would make him a formidable foe against Ladybug and Ichigo.
A powerful and evil dragon could be the main antagonist. This dragon might have a grudge against the dragon slayers in general and specifically targets Lucy because of her growing reputation as a star dragon slayer.
It could be an evil ice dragon that has gone mad with power. This dragon might be hoarding all the ice magic in the land, causing problems for the people and other magical creatures. Lucy would then have to face this powerful foe to restore balance.