Correction on the ABIT KT333 motherboards:
There are two of them: the "legacy-free" motherboard (with an AGP slot and only three PCI slots, and with onboard audio, LAN, and four-channel UATA133-RAID - which brings the total IDE-device capacity to 12) is the AT7 MAX; the conventional one (with no onboard audio or LAN but offers the option of an integrated UATA133-RAID controller, and has an AGP slot and six PCI slots) is the KX7-333(R) (the "R" signifies RAID). I was wrong on the AT7 MAX being a uATX form factor; in fact, both ABIT KT333 boards are standard ATX form factor. And both ABIT boards have four DDR333/PC2700-compatible DIMM slots, but keep in mind that the KT333 chipset itself officially supports only four RAS lines of memory at DDR333/PC2700 speed. In other words, you can only use two double-sided DDR333 modules OR one double-sided DDR333 module plus two single-sided DDR333 modules OR four single-sided DDR333 modules.
And going back to "Which to upgrade?", I upgraded both my computer and my headphones. (Well, not full-sized headphones, anyway, but bought the amazing Etymotic canalphones.) But that took me over 10 months since I first asked this question. My PC is now configured with an AMD Athlon XP 1600+ processor, 512MB of DDR266/PC2100 DDR SDRAM memory, an ABIT KR7A-133 (no RAID) motherboard with a VIA KT266A chipset, a 120GB WD1200BB (not JB) HD, a Built By ATI Radeon 8500 64MB Retail video card (my older Radeon 64MB DDR VIVO card crapped out because it wouldn't hold its geometry, position or size settings for long - it would often reset to factory defaults
oooooyeeeeuuck!
), a Turtle Beach Santa Cruz sound card (no more craptacular bloated Creative driver kits - YAY!
) - and (in addition to my current 8x DVD/40x CD-ROM drive) a 24/10/40x CD-RW drive. I think my next upgrade will definitely be the addition of a decent dedicated headphone amp, and possibly one more set of full-sized headphones (I'm thinking of AKG K501, Beyerdynamic DT250-80, Sennheiser HD 580 or HD600).