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So, just to set things straight - if I use MP3Gain, would I have to turn on Sound Check in iTunes and on my iPod?
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If you use MP3Gain in Track mode then no, you wouldn't have to use Soundcheck. You'll find that MP3Gain is far better than Soundcheck which still seems to vary the volume of tracks quite considerably.
If you use MP3Gain in Album mode but still decide you want to sometimes have everything playback at the same volume then you would use Soundcheck as well.