Playing blu-rays, with the radeon is pretty much bit perfect, so you should do as much calibration in the TV as possible.
What you can't calibrate out of the TV can be compensated for with calibration of the video card. Any of the PC calibration products can work, my favorite of course is CalPC, but that's probably only because I help write it. I do think CalPC will give you the most accurate grayscale calibration of any PC calibration software. It's ICC utility isn't as powerful as something like BasICColor, but ICC's aren't usefull for HTPC use anyway.
CalMAN Lead Developer