Why is pinning down the character's alignment necessary?
For the purpose of Detect Alignment things. He acts nice most of the time, but If the paladin uses detect evil, I need to figure out what he senses.
I would say he senses an evil psychopath. The character you are describing sounds like a crazy person (which you admit to) who knowingly does evil acts for an assumed good that he believes happens, but never actually sees the fruits of. The thing about games that use alignment rules is that good and evil sort of stop being philosophical concepts and become measurable quantities. If you knowing do evil, you are evil.
Your NPC may be misguided in his evil ways, or maybe he's not wrong for doing evil for whatever reason he does it, but he's doing evil on the side of
Evil and expecting the manifestations of
Good to sort of pick up the slack (without much proof that it even can beyond his own belief). And he's not indiscriminately being evil either, he's got rules, structure, codes of conduct in his evil to maximize the output of imagined good elsewhere. He's rather lawful in that respect.
Anyway, long story short, your dude is Lawful Evil.