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As I understand it at the moment Calibre assumes the Python 2.6 series (with the current latest release being 2.6.2). There are significant language changes between the 2.6 and 3.x series, so I would not be sure that Calibre would compile correctly with 3.1 (although I guess I could be wrong).
Also as Kovid mentions, at the moment the 3.x series is measurably slower than the 2.6 series of python.
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