Ok... from the top. My opinions as a long-time D&D and league player. I might elaborate on some. Post one of two, since this went LONG.
- Chaotic Neutral. Brings or drags out bloody war, but has no real malice in him. He's pretty beyond ideas of morality in general.
- Chaotic Neutral. Acts on whim and her own desires. Her recent development of a conscience means SLIGHT good leanings.
- Lawful Neutral. Obeys her order and Shen. Has a fierce dark streak and favors punishment over redemption, but not a sadist or bully.
- Chaotic Good. Hard to peg him, but he's an escaped slave, so probably values his independence a LOT. Definitely good tho.
- Neutral Good. Innocent and friendly, but very immature and with a temper. Bears no one real malice, but often hurts people accidentally.
- Chaotic Good. Above laws and authority, but compassionate and kind.
- Chaotic Neutral. Bratty, slightly spoiled child. Does what she wants. Seems like she could EASILY become evil over time if she stays selfish.
- Lawful Good. A leader and a speaker for peace and unity. PRETTY clear cut.
- True Neutral. Disinterested in pretty much everything on runeterra but not malicious. Kind of a dick, tho.
- Lawful Neutral. He's the emperor and the emperor demands obedience. Might be slipping towards good after the whole slave thing.
- Chaotic Neutral. Does what it wants, when it wants, for reasons it wants.
- Neutral Good. Big, friendly robot. Might even be lawful good, but I see him as more of a "help your neighbors" kinda guy.
- Chaotic Evil. Some men just want to watch the world burn.
- Neutral Good. It's freaking Braum. He's like, the goodest guy in the setting.
- Lawful Good. She's a cop, she helps and protects people as best she can and is trying to clean up her hometown.
- Neutral Evil. Selfish, manipulative and LITERALLY a backstabber. Pretty clear cut.
- Neutral Evil. Probably. Void monsters are alien and unfathomable but "eat everything and laugh" is pretty evil, so...
- Lawful Mustache. Oh, I mean good. Sorry.
- Lawful Evil. Might makes right. The strong should rule. Power above all? Textbook Lawful Evil.
- Originally Chaotic Good. This one was hard. If she really wants to kill the sun over a vendetta against a few old men who mistreated her, she's pretty spiteful and probably CE. Also crazy. If she's all talk and not a bad person to anyone who DIDN'T betray her, she could be CN or even CG.
- Chaotic Evil. You won't like him when he's angry.
- Chaotic Evil. But oh-so charming. Seriously tho, man murders people for attention and is entirely self-obsessed.
- Chaotic Overpowered.
- Neutral Evil. She feeds people to a giant spider to stay young.
- Neutral Evil. Probably. Her lore is vague as hell, but she's definitely a bit of a sadist, so probably evil.
- Chaotic Good. Does his own thing and makes his own rules, but seems like a good guy.
- Neutral Evil. Er... probably? He's so alien and mysterious it's hard to really say what motivates him.
- True Neutral? Fiora is hard to peg. She broke social custom but for personal reasons and doesn't really seem chaotic overall. She's a half-decent person but more interested in her family's well-being than defending the innocent or anything. She could fit a few alignments, but I'll put her as TN.
- CHAOTIC EVIL. Ah, but seriously... I hate this little jerk. In the lore he's probably Chaotic Neutral though. Maybe even Chaotic Good.
- Lawful Good. A guardian who protects others. Hard to peg him as much else.
- Neutral Evil. With chaotic leanings. A brutal, violent man who acts even MORE brutal and violent to keep people in line.
- Lawful Neutral. Considers himself lawful good, but he's a zealot of his nation not a paladin. "What we do is right!". Not always, Garen.
- True Neutral. Basically a very smart animal. Doesn't really have any morality one way or the other.
- Chaotic Neutral. Get drunk and punch things. Yep... sounds about right.
- True Neutral. Values loyalty to his running crew but otherwise a thug, con man and a criminal.
- Neutral Evil. Also, kind of a jerk.
- True Neutral. Possibly neutral good if you want to say his motivation for invention is to better the lives of everyone he can. He... mostly seems to invent guns and rockets though, so I think it's more about just liking to build stuff.
- Chaotic Evil. Her philosophy is basically "rampant hedonism + take what you want". MAYBE you can call her CN, but she basically teaches the kind of mindset that encourages sadists to torture, bullies to abuse others and rapists to... well... Plus she supported GP and he's evil as sin.
- Lawful Neutral. Good leanings but more a patriot than a paladin, a lot like Garen.
- Chaotic Neutral. Fickle and flighty like the wind.
- Lawful Neutral. This one is hard, but I'll put him LN like Garen. He's about his country, right or wrong.
- True Neutral? Has no real lore to speak of, so this one is pretty impossible to say one way or the other.
- Lawful Good. Wants to help people, bring prosperity and ensure a better future. Kinda comes off as a smug jerk tho.
- CRAZY. Jhin is mentally ill in so many ways. He kills people for pleasure, realizes it's wrong, feels guilty... convinces himself it's for art... wears a mask because he hates his own reflection... Deeply, DEEPLY disturbed dude. Probably Neutral Evil if we have to ascribe an alignment to him.
- Chaotic Evil. ALSO crazy, and far, FAR more erratic than Jhin. Still kills people plenty in "depraved indifference" kinda way. I don't care if they want to call her CN, if you're entirely in life for kicks and you get your kicks shooting people and blowing up stuff, you're evil. She KNOWS she's killing people, she says so in many of her lines... she just doesn't care.
- Lawful Evil. Vindictive, angry and just as prone to cursing people as the other shadow isles champs. At least she's honorable?
- Lawful Good. Possible argument for her being LN like Irelia, but I think she's more about compassion than valor and honor.
- Neutral Evil. Possibly even CHAOTIC evil. He murders things for the heck of it because he's obsessed with death.
- True Neutral. I don't know Kass's lore SUPER well, but I think he's more about stopping the void than worrying about what he has to do to accomplish that. If he had to murder a pile of innocent kids to seal a void portal, I think he would consider it a necessary evil. If not, he's prob NG or CG.
- Neutral Evil. Possibly CE, even. An assassin without remorse, but too loyal for me to consider her chaotic, despite her thrill-seeking and reckless actions. Her emotional nature (PASSION!) and chaotic side keep her from being a lawful evil sort like many of her fellow Noxus champs tho.
- Lawful Lawful. In all seriousness, Kayle is either lawful good (emphasis lawful) or lawful neutral, depending on how much truth there is to Morgana's cries of Kayle being an oppressive, fascist templar without remorse. In either case she is RIGIDLY lawful though. If Aethyr Wing Kayle is any indicator she's die-hard oppressive Lawful Neutral with shades of Lawful Evil. Skins aren't really cannon though.
- Lawful Good. Loyal, honorable and oathbound to follow his order and Shen, but consistently described as merciful and forgiving.
- Neutral Evil. By our silly, mortal reasonings, anyways. Void creatures don't really follow any human codes of morality.
- True Neutral. They're personifications of death. Blaming them for killing things is like blaming fire for being hot. Wolf is essentially a big, dumb animal and Lamb is serene and seemingly gentle. Neither kills out of spite or hatred. Wolf enjoys it a bit much, but still...
- True Neutral. In the sense that he's essentially a huge, dumb infant. He's too immature for morality of any sort.
- Neutral Evil. Probably. If she IS in fact loyal to the Black Rose or Noxus as a whole you could argue she's Lawful Evil easily enough.
- Lawful Buddhist... er, good. The man set himself on fire as a means of protesting an injustice. He's all about self-sacrifice and atonement.
- OLD Leona was Lawful Good. NEW Leona is awful. I'll stick with old Leona, the peaceful but stalwart defender of the weak.
- Neutral Evil. Pretty typical manipulative, evil witch. She is planning to betray all her "friends" and give the world to the watchers, so... yeah.
- Lawful Good. But REALLY obsessive with his task. In a pinch I think he'd protect people and give his life for it, but he's so focused on his revenge that he's not really helping people out as much as he is obsessively trying to kill monsters... thresh especially. Probably has a deathwish too.
- Chaotic Neutral. She LITERALLY has a spell called whimsy. Too easy. NEXT.
- Lawful Good. POSSIBLY LN like her brother tho. She does her job out of obligation (lawful) but secretly yearns to be CG and make her own choices in her life. This is probably why the canon is Lux x Ezreal. He's everything she wants to be and he... um... needs a beard to squash that "Taric rumor".