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Accel World comes to mind for me. With the writer of Guilty Crown and an initially wussy weak willed character voiced by the then incredibly typecast and thus played out Yuki Kaji I didn't expect to last more than a couple eps of fancy with this. Instead I found myself getting pulled into a well produced adaptation with one of the most ambitious yet well rounded and not to mention gorgeous and elegant heroines I'd seen in ages. The show also doesn't get nearly enough credit for its ensemble cast which at times can get overshadowed by said heroines "presence", but theyre all pretty enjoyable and get there moment in the spotlight. Was not expecting this to be anywhere near as enjoyable as it was let alone enjoyable at all so yeah it takes the cake.
Honorable mentions:
Zetsuen no Tempest (actual coherent Bones show for 2 whole months now)
Muv-Luv Alternative: Total Eclipse
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