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Homemade sources tend to take a real quality beating when run through DVD Shrink. DVD-Rebuilder may be a better option, as it full re-encodes the video.
Starting over may also be a good solution.
You have to carefully watch your file size.
On the other hand, it may be time to just admit defeat on this one disc, and burn to DVD+R DL instead, and be more careful next time, if your goal is to fit everything onto single-layer discs.
Beyond all this, 4.2GB is filesize, not bitrate. Not the same thing.
You seem to be having several unrelated issues. You'll just need to muddle through it and hope for the best.
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