There's something to be said for having everything with you and not having to worry about grabbing it off a computer when the urge/need hits, provided you're even near your library at that time. That can be somewhat addressed by having a copy stored in the cloud (provided your cloud provider works with your device of choice and you have an internet connection), but I find I'm happiest when I have everything at hand.
I really wish there was something like Calibre Companion for iOS.
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