In this fanfiction, Harry could gain the power of enhanced perception. This would allow him to see things that normal humans or even wizards can't, such as the flow of spiritual energy. He might also gain the power to transform into a more powerful form, like a Shinigami's Bankai. His existing magical powers could potentially merge with his new Shinigami powers, creating something entirely unique. For instance, he could use his Patronus charm in a new way within the Shinigami world, perhaps as a form of spiritual protection.
First off, Harry Potter would be quite disoriented in the Shinigami world. However, his inquisitive nature would drive him to explore. He'd likely start by observing the Shinigami at work. He could draw on his knowledge of the wizarding world's laws and ethics to understand the Shinigami's code. His ability to think on his feet, which he developed during his battles against the Death Eaters, would be useful when he has to make quick decisions in the Shinigami world. For example, when deciding whether to purify a Hollow or not.
One challenge could be controlling his new powers. Deadpool's powers are quite wild, and Harry, used to more traditional magic, might struggle to master them. Another challenge could be how the wizarding world views him. His new powers and the resulting change in his behavior might make him an outcast among some in the wizarding community.
Harry might gain the ability to dodge attacks more easily. Sans has a certain 'instinct' for avoiding harm, and if Harry had this, it would be much harder for his enemies to land a hit on him. This would be really useful in duels, especially against powerful dark wizards. It could also make his Quidditch playing even more amazing as he could dodge bludgers effortlessly.
In the fanfiction, Harry Potter might gain the power of precise control. The Nuibari is known for its ability to stitch things together in the original Naruto context. So perhaps Harry could use it to 'stitch' spells together in a new and unique way, creating more powerful and complex incantations.
It could be that he has been wronged by the wizarding society. So, in a form of rebellion, he decides to become a thief. He might steal from those who he thinks are corrupt or unfair. For example, if the Ministry of Magic has been unjust to him or his loved ones, he could target them or their allies. Another possibility is that he is influenced by a powerful and devious character who convinces him that stealing is a way to gain power or freedom.
He could gain the power to control time, which would be really useful in the wizarding world. He could go back and prevent some of the bad things that happened, like the death of his parents.
The plot could start with Harry having strange dreams about Shinigami. As he investigates, he discovers that there is a hidden portal in Hogwarts that leads to a realm where Shinigami exist. He and his friends enter this realm, and they find out that there is a dark force in the wizarding world that is related to the Shinigami in some way. They then have to work with some friendly Shinigami to stop this dark force. Along the way, they learn about new forms of magic and the true nature of death from the Shinigami.
It could be Spider - Man. Harry Potter might relate to Peter Parker's journey of having great power and great responsibility. Just as Harry has to deal with his own powers as a wizard and the burden of saving the wizarding world, Peter has to balance his normal life with his superhero duties.
Perhaps some of the magical creatures that Harry has befriended over the years, like the centaurs or the house - elves, could become his allies. They could offer their unique skills and knowledge to help Harry in his new role, and Harry, in turn, could work towards better rights and treatment for them in the wizarding world.
Another possibility is that he becomes a fox. Foxes are clever and sly, which are qualities that Harry has developed over the years. As a fox, he could use his wits to outsmart his opponents. He could also easily blend into the forest environment, which would be handy for hiding or sneaking around.