That's a tough one. Each one would come down to toughest single album to get. Of the Columbia ones, Famicle Parodic 2 is the one that notoriously hard to find. You'd also probably have a tough time finding Fire Pro Wrestling Combination Tag and Insector X. The others strike me as being potentially expensive (especially Super Mario Land and Chikudenya Toubei), but not necessarily hard to find. I am missing 7 of that set.
As for the Tokuma collection, they all seem to be really hard to find. I've been buying VGM for almost 20 years, and I've never seen an auction for Chachamaru Game Music or Fire Pro Wrestling 2nd Bout (not that I have been continually looking). I got 5 of these albums in one lot about 10 years ago, and was fortunate to find another forum member selling a few others. F-Zero is readily available, and CD Technopolis and Masaya Omnibus are probably the next easiest ones in that set to find, but the others are a beast. I won an auction for Devil's Crush once, and the seller never shipped it. I think it took about a year to find another copy. At this point, the only one I'm missing is F-Zero, but some of my copies are incomplete.
So, I'd say it's easiest to get an almost compete set of the Columbia albums. For the totally complete set, I'd say it's probably equally difficult because Famicle Parodic 2 and Chachamaru Game Music are both so difficult to find.
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