This can be interesting.

FF:
Warriors of Light - Lawful Good
Four Fiends - Lawful Evil
Chaos - Neutral Evil

FFII:
Firion and most of the cast: Lawful Good
Leilei - Lawful Neutral
Leon - Lawful Evil
Emperor Mateus - Lawful Evil

FFIII:
Onion Knights - Lawful Good
Unie and Doga - Neutral Good
Xande - Neutral Evil
Cloud of Darkness: Lawful Neutral

FFIV:
Cecil - Begins Lawful Neutral, become Lawful Good
Kain - Lawful Neutral, when brainwashed, he's Lawful Evil.
Rydia - Neutral Good
Tellah - Chaotic Good
Edward - Lawful Good
Rosa - Lawful Good
Yang - Lawful Good
Cid - Chaotic Good
Edge - Chaotic Good
Palom - Chaotic Good
Porom - Lawful Good
FuSoYa - Lawful Good
Golbez - Lawful Evil
Elemental Archfiends - All Neutral Evil except...
Rubicante - Lawful Evil
Zemus - Neutral Evil
Zeromus - Chaotic Evil

FFV:
Bartz - Chaotic Good
Lenna - Lawful Good
Faris - Chaotic Neutral at first becomes Chaotic Good later
Galuf - Neutral Good
Krile - Lawful Good
Gilgamesh - Chaotic Neutral
Exdeath - Neutral Evil
Neo Exdeath - Chaotic Evil

FFVI:
Terra - Neutral Good, becomes Lawful Good
Locke - Chaotic Good
Edgar - Neutral Good
Sabin - Neutral Good
Cyan - Lawful Good
Shadow - Chaotic Neutral
Gau - Chaotic Neutral
Celes - Lawful Good
Mog - Neutral Good
Strago - Lawful Good
Relm - Neutral Good
Umaro - Neutral
Gogo - Neutral
Leo - Lawful Good
Banon - Lawful Good
Cid - Lawful Neutral, becomes Neutral Good
Gestahl - Lawful Evil
Ultros - Neutral Evil
Kefka - Chaotic Evil

FFVII:
Cloud - Neutral, becomes Neutral Good
Barret - Chaotic Neutral, settles down to Neutral good.
Tifa - Lawful Good
Aerith Neutral Good
Red XIII - Neutral Good, then becomes Lawful Good
Cait Sith - Lawful Neutral/Lawful Good
Cid - Chaotic Good
Yuffie - Chaotic Neutral
Vincent - Lawful Neutral
President Shinra, Heidegger, Scarlet, Palmer, and Rufus - Neutral Evil
Hojo - Chaotic Evil
Reno and Rude - Neutral
Elena and Tseng - Lawful Neutral
Jenova - Neutral Evil
Sephiroth - Neutral Evil, occasionally slips in Chaotic Evil

FFVIII:
Squall - Lawful Neutral then becomes Lawful Good
Laguna and his crew are Neutral Good
Sqaull's companions are Lawful Good
Seifer - Chaotic Neutral
Fujin and Raijin - Chaotic Good
Cid - Neutral Good
Edea - Lawful Good when not possessed
Ellone: Lawful Good
Dr. Odine - Chaotic Neutral
Biggs and Wedge - Lawful Neutral
Adel and Ultimecia - Neutral Evil

FFIX:
Zidane, along with all of Tantalus - Chaotic Good
Ganet - Neutral Good
Steiner Lawful Good
Vivi - Lawful Good
Freya - Neutral Good
Quina - Neutral
Eiko - Chaotic Good
Amarant - Chaotic Neutral
Zorn and Thorn - Neutral Evil
Queen Brahne - Neutral Evil
Garland - Lawful Evil
Kuja - Neutral Evil turned Chaotic Evil.

FFX:
Tidus - Chaotic Good
Yuna, Wakka, Lulu and all of the "good" NPCs - Lawful Good
Auron - Chaotic Good
Rikku - Neutral Good
Seymour - Runs the gambit of all three Evil alignments depending on where you are in the plot.
Jecht - Chaotic Good
Yu-Yevon and most of the "evil" NPCs - Lawful Evil

FFXII:
Vaan - Chaotic Good
Penelo - Lawful Good
Balthier - Likes to think he's Chaotic Neutral but he's Chaotic Good
Fran - Chaotic Good
Basche - Lawful Good
Lady Ashe - Lawful Neutral but becomes Lawful Good
Gabranth - Lawful Evil, becomes Lawful Neutral
Drace - Lawful Good
Bergen - Chaotic Evil
Zargabanth - Lawful Neutral
Ghis - Lawful Evil
Vayne - Lawful Evil
Cid - Chaotic Neutral
Venat - Chaotic Neutral
The Occurians - Lawful Evil

FFXIII:
Lightning - Lawful Neutral
Snow - Chaotic Good
Sahz - Neutral Good
Hope - Lawful Good
Vanille - Neutral Good
Fang - Neutral Good
Cid - Neutral Good
Rosch - Lawful Neutral
Jihl - Lawful Evil
Barhtandalus - Lawful Evil
Orphan - Neutral Evil.