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Maria-sama is my favourite in the shoujo-ai category. Probably because it's very subtle and not (generally) in your face. Has a solid story and is an enjoyable school-life series.
Surprised nobody's mentioned Mai-Hime (and Otome) yet. While the leading romance is straight, there are very strong shoujo-ai vibes in many pairings, and one open one. Not to mention it's an enjoyable action/magic girl franchise. (the OVAs included)
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