In my book:

Lae'zel - lawful evil. She has a code honor that all githyanki share. She's absolutely loyal to her lich queen Vlaakith. And she's not a liar. Hence her lawfulness.
Shadowheart - neutral evil.
Astarion - chaotic evil/neutral. I gave him neutral cause it's absolutely dependent on how you treat him. He's all about survival, living in the now and having some fun while at it. Also enjoys some blood shed.
Gale - true neutral/neutral good, possibly. Could be a stretch.
Wyll - chaotic good. Anything is justified for the greater good kind of character.