Which game has your favorite selection of shot types?
I'm not sure if that's the best way to phrase it, but I'm referring to the entire range of shot types in a game-- don't pick a game just because you really like one shot type from it.
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I'd go with either SA or DDC. While they're certainly not balanced, both games have some nice variety to their shot types, including some rather weird (and therefore memorable) abilities. For example, SA has ReimuA's gapping (and graze bomb), ReimuC's super-speed (though the aiming and bomb power are more relevant), MarisaA's bomb system and reversed focus/unfocus, and MarisaB's five-element selection; DDC has ReimuA's crazy gohei, SakuyaA's time slow, MarisaB's constant power items, and SakuyaB the weak high-scoring character. They also have rather distinct bombs that mostly have their own uses, particularly for scoring.