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Is there any good reason that I need to wait for iTunes to give me permission to remove an iPod from my computer?

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Yes. It's possible not all the writes to the device have completed. It's possible you may leave the filesystem in an inconsistent state, corrupting it.

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Yup. Same principle applies to flash drives or any removable devices - don't remove the drive until all writes have finished. – WindowsEscapist Dec 26 '12 at 3:18

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