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Given that a nationally representative body had already weighed in on [tarriffs], it doesn't seem unreasonable that the South would have to then appeal to the next logical means of asserting their rights.

Well that's where we disagree I think. If on the one hand you acknowledge that the national government HAS the right to set tariffs, then you can't on the other hand assert the states' rights to violently resist them. E Pluribus Unum.

That is why I say they resorted to anarchy. Republicanism depends on the parties all honoring their obligation to the compact. Now, can we say that certain policies were obnoxious to the spirit of Union? Most definitely. We could say certain tariffs were obnoxious to southern interests, just as we could say the Fugitive slave laws were obnoxious to certain northern interests. And so on. In fact, the most accurate historical descriptions of American politics of that era speak of "sectionalism":

"These opposite economic arguments furnished agitators on each side abundant ammunition for rhetorical exercises in reciprocal denunciation. When submitted to scientific analysis, such arguments will be found to consist partly of solid truth and partly of fallacy. It was true that the South had an essentially colonial economy, from which heavy profits were drained off by Northern middlemen. It was also true that Southern political power, disproportionate to the sections economic strength, helped retard measures which Northern capitalists desired. Yet the Southerner usually erred in refusing to admit that the North was making a major contribution to the Southern economy, while the Northerner often failed to see how much of his profits depended upon the Southern trade. Those Southerners who demanded separation for economic reasons were not thinking sufficiently in terms of mutual dependence. Even if separation should come, yet physically, as Lincoln said, the sections could not separate: they would have to go on living side by side; and the many elements of economic interdependence would continue to operate."
From www.civilwarhome.com

From the standpoint of a republican, the question becomes this: Was the Revolution fought over the issue of taxation? Or taxation without representation? I believe it was the latter. No tariff, no obnoxious pamphleteers agitating slave insurrection, no regulation of slavery in DC is cause for revolution against the United States. That's not reasonable.