i am far from an expert, but i can try

honestly i feel like i’d put crowley more as chaotic good. yes, he’s a demon. sure, he does bad things. but that’s just because it’s what he’s supposed to do. at heart, if left alone, he just really cares about people and wants to do what’s best. (and maybe cause some mischief along the way, but hey, what’s the point of living if you can’t have some fun?)

aziraphale is harder? i’d say by inclination he’s more chaotic, but he’s trying to be lawful good. he thinks he wants to follow the rules. and he thinks heaven’s rules should be good. but the moment he sees a rule he dislikes he breaks it! gives away his sword, makes deals with demons and does half their homework. so at the beginning of the series this maybe averages out to a neutral, but by the end he’s let go of expectations and gone full chaotic. book aziraphale maybe leans more towards true neutral, but i feel the tv version i’d also put as chaotic good

the thing with aziraphale and crowley is that, more than anything else, they’re motivated by love. love for earth. love for humans and all the ridiculous and wonderful things they can do. love for each other. being an angel and demon is just their job, and not one either especially cares for. they do it because they have to, but they’d much rather just hang around earth having fun

gabriel is definitely lawful evil who thinks he’s lawful good. honestly most of the angels we see seem to fit this

hastur is absolutely evil, but i don’t think i’d call him lawful? though hell’s whole thing being chaos makes it a bit weirder to categorize. possibly more neutral, since while he’s doing what he’s ordered, he’s also got his whole hastur la vista thing. beelzebub maybe would be lawful evil

the horsepeople probably all fall in neutral, rather than good or evil. they are things that exist, but not out of their own malicious intent. death, perhaps, lawful neutral, famine true neutral, war and pollution chaotic neutral

adam, sort of by definition, is the most true neutral of all. not good, not evil, not heaven, not hell, just human. the rest of the Them possibly also fall here? mostly i feel they’re too small to really be firmly anywhere

anathema is maybe lawful verging on neutral good, if the laws you follow are agnes’ prophesies, and by throwing those off in the end, pushes herself more to neutral. newt is...idk, i don’t care enough about newt to have thought about him much. neutral good? true neutral?

shadwell is chaotic neutral/evil. sure they try to make him seem endearing in a weird old man way, but literally every other thing he says is calling someone a slur, and that is. not actually forgivable in my book. madame tracy i would put as neutral good

i have to go through them all and edit them later, & i’ll post more on here later too, but here are a couple for now 😎👍