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I believe the Volt's drivetrain is similar to the Prius' in that it has separate electric and gasoline motors. Except instead of running electric from 0-20 (or whatever) it just runs all electric till it runs out of juice, then switches over to the gas engine completely.
What you're referring to, though, is a serial hybrid like they use in diesel train engines. I've seen a few attempts at homebrew serial hybrids and apparently they're pretty complex electronically, and pretty expensive for the right components.
If you can do it, go for it! Get your google on and you should be able to pick up some good info.
*edit* - though I could be wrong about the Volt drivetrain, their propaganda is pretty vague.
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