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In addition to theducks' suggestions:
1) You updated your antivirus/"Security suite" and it now doesn't like calibre.
2) You updated from Malwarebytes Free to Malwarebytes (not free). The not free version blocks calibre's network connections.
3) You updated your device to Android 4.4 (kitkat) and your library is on an SD card.
Basically, something changed and you need to determine what that "something" is. Some candidates are new routers on your network, anti-virus/security suites on the machine running calibre, changes to your device (new apps, security suites, version of android).
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