(Warning, spoilers below for companion development)
Okay, Okay, before everyone yells at me: Let me explain.

1) I know there is no alignment in the game. Got it.
2) I know alignement threads can get super heated and devolve into shouting matches, I don't want that.
3) I know everyone's take on alignment is differrent.
4) I'm aware thare are probably 11 babillion versions of this thread so far.

I got all that.
This is just a fun little thought exercise about how my brain works. It is not meant to be taken seriously. If you disagree, please put down your kind and thoughtful words in the comments below. No need to start a flame war.

First of all, the way I envision alignment is:
Good is selfless, willing to help others, and having a respect for life (especially sentient life.) Does that mean you won't kill? No, it means you don't like killing.
Evil is selfish, drivin by profit or greed, and having no respect/contempt for other life.
Lawful is being orderly (not nessissarily following the law) . Lawful characters tend to have a code of conduct that they follow, try to plan out their actions, and generally don't like flying by the seat of their pants.
Chaotic characters enjoy freedom, they like going with their 'gut feeling' and having the liberty to change their minds. They generally think plans are boring and have trouble sticking to one thing for a large amount of time.

So with that in mind:
Lae'Zel: I think Lae'Zel is Lawful neutral, leaning lawful evil. She does have a contempt for other living creatures, but that's not from malice, that's the Gith brainwashing literally telling her other species are stupid and worthless. She is VERY dedicated to her Gith code, making her lawful, but I hesitate to say she is outright evil because, she isn't doing what she's doing out of perverse pleasure or to gain power . . . she just thinks that's how things should be done.

Shadowheart I'd peg as True Neutral, leaning slightly neutral good. She doesn't seem to have strong convictions and takes things as they come. She is okay forming plans or discarding them if they don't work out, meaning she's not really lawful or chaotic. Her god preaches a lot of evil stuff, but she ends up okay saving the tieflings if you do that, and kinda-sorta-halfheartedly says she'll apologize to Shar for helping people later. To me this puts her slightly on the good side of neutral for me.

Asterion is Neutral Evil, but only just. Like Shadowheart he doesn't mind a plan but doesn't get his heart set on things, and he has a loose personal code (that is, get money, save yourself.) So I think he's neutral on the law-chaos spectrum. He's all about self-survival and getting the most out of any deal, pretty selfish, (not to mention getting out from under the thumb of his master,) but he admits that he isn't adverse to helping people once he's in a position of power. So I think he's NE boardering on TN

Gale: To me, Gale is Neutral Good, bordering on Chaotic. He clearly enjoys helping people, like the tiefling child in the druid grove (reminds him of when he was her age) and routing the goblins to help the tieflings. This puts him in good on my book. Like Shadowheart he seems okay making plans or abandoning them, but the real issue here is how reckless he was with his backstory and getting the piece of the weave. Obviously it was a youthful indiscretion, but I'm not convinced he wouldn't do it again.

Wyll: Solid Chaotic Good, though with a slight dip towards chaotic neutral. He's all about helping people and boasting and bragging. He seems to not care about plans at all and will attack evil goblins on site even if he is greatly outnumbered. This all screams chaotic good, though his blind hatred for goblins and inability to entertain that there could be a good goblin does ding his alignment towards evil a little in my book.