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Even when Philip first entered the Boiling Isles, he was a bit bitter about how his brother left him behind in Gravesfield. Still, he was willing to put that aside in the hopes that he could make everything go back to normal. He would find his brother again and would make sure to triumph over witches once more.
But even back then, in the lonely hours of the night, Philip couldn't help but think of the possibility that Caleb didn't want things to go back to normal, that he actually liked the Boiling Isles for some godforsaken reason. He knew his brother really enjoyed the company of that one witch Evelyn. It made him jealous. Why was she so great?! What did she offer that he didn't? She was the enemy!
Philip cried some nights, wondering if he could still pull on his brother's heartstrings like when he was younger. He found comfort wallowing in pain and suffering, crafting a story of how difficult it was for him to be all alone for so many years, conveniently ignoring how most of the pain and suffering was self-inflicted. The people of the Boiling Isles were primarily kind and welcoming, even if they didn't understand him, but Philip did not want to reciprocate. His actions repeatedly gave him a bad reputation, causing townsfolk to become weary of him. But Philip never was honest with himself about this. He thought himself to be wrongfully ostracized.
When Philip actually confronted his brother, he learned his worst nightmares came true. Caleb not only enjoyed the Boiling Isles but he loved Evelyn. She was pregnant with his child!!! This infuriated Philip to no end, to think that Caleb left his real family behind just to make a new one! Of course, Philip conveniently ignored Caleb's genuine apology and willingness to make amends in the form of welcoming him into part of his family. But Philip couldn't do that. Accepting these witches was something he refused to ever do.
He told himself that his brother was brainwashed by Evelyn despite knowing she could do no such thing. Caleb loved Evelyn and the Boiling Isles on his own accord and there was nothing he could do about it. He ended Caleb's life out of frustration and anger that he would never have it his way and to bring pain to Evelyn. In his eyes, the suffering of witches was more important than his brother's own happiness if his brother's happiness did not come from him.
As Philip began his actions to "vindicate" his brother, becoming Belos and starting to make grimwalkers, he'd sometimes think about hypothetical situations where Caleb would take his side, that he'd turn on Evelyn and work alongside him to eradicate all the witches of the Boiling Isles. But he know Caleb was never like that. He was always a bit hesitant of witch hunting, even back in Gravesfield, and in reality, there was no way to make him more comfortable with the concept.
Philip never understood why Caleb hated witch hunting so much. It probably had something to do with how caring he always was. Philip always disliked that about him. He'd tried to help little animals and the other townsfolk and not pay attention to his younger brother. Philip would try to get his attention, to "cry wolf" so to speak, but Caleb grew frustrated. Of course, Philip never really acknowledged that Caleb was his own person and was free to do as he wished, even if he didn't approve.
Still, as Philip became Belos, he'd tell himself that he tried to save his brother's soul from witchcraft and killing him was the only option. Never once did Philip try to save his own soul from self-inflicted pain, from his own victimization that kept him mentally trapped in the same place for hundreds of years. He may have traveled to the Boiling Isles after being left behind by Caleb, but he never made the effort to mentally move on from the thought that he was the victimized abandoned younger brother.