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You aren't running a big 12 volt load off of one battery are you? That will also cause an imbalance.

The first thing I would do is measure the voltage across each battery. If it is less than 12.6, I would slow charge it. Once they read 12.8, I would start the vehicle and measure it again. You should see less than 15 volts across each and they should be about the same. A sudden high...