It doesn't appear that Thomas Jefferson would take an "either or" approach. Nullification wouldn't replace the option to succeed, rather it would be the first step before succession:
From Wikipedia (http://en.wikipedia.org/wiki/Alien_and_Sedition_Acts):
"Jefferson and James Madison also secretly drafted the Kentucky and Virginia Resolutions denouncing the federal legislation, though state legislatures rejected these resolutions. Though the resolutions followed the "interposition" approach of James Madison, Jefferson advocated nullification and at one point drafted a threat for Kentucky to secede. Jefferson's biographer Dumas Malone argued that this might have gotten Jefferson impeached for treason, had his actions become known at the time."
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