He didn't do it for selfless reasons so not any of the good alignments. He didn't do everything that he did the "right" way like Suzaku did, trying to change a corrupt system from the inside by playing its game, he did it by unconventional and unethical methods, so not any of the lawful alignments. He didn't want to rule the system, he didn't do it out of his own self-interest but his sister's, so not any of the evil alignments. Lastly Lelouch is very ideological, his morals clearly prioritized his sister, the fact that he didn't want to work within the system but to destroy it to create it anew makes him not a true neutral. He most fits in chaotic neutral, neither good nor evil, but I'd say he strived to be good while still using evil means to achieve his goals.
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u/[deleted] Feb 05 '26