I don't have any experience with ATI cards, I've stuck to the green side of the fence for my setups... But 66C doesn't sound like anything to be worried about. I would probably only start worrying if it gets close to 80C or 90C. Maybe someone with some experience OC'ing ATIs could be of more help though.
Otherwise, you could probably find tons of helpful info on your card on the Overclock.net forums... Obviously though, we'd want to hear all about it afterwards.
I will admit, I was an avid Nvidia fanboy once upon a time, in my mind it was the one and only option, I was gonna get an x80 and that was that. By the time I had my money together though, the situation changed a little. I eagerly awaited Nvidia's new cards, now too close for me to want a 580, however with speculation of them being as far off as september 2012 on some sites, I grew impatient. Then AMD released their 7xxx series and my money called to me, it begged to be let out

. I went for it and got my 7950, it was a month or two before the 680 came out, but it would have been out of my price range anyway.
I've been impressed with its performance, I am a little gutted its now like $100 cheaper, but hey, for 2 months I had one of the most powerful graphics cards on the planet, a great step up from my geforce 210 nearing its 1st anniversary (yeah I only entered the custom computer circle about 15 months ago).
Back to nowadays, I did several more consecutive tests, at the end I did a 15 minute burn in test with furmark on extreme settings, it held at 69C for about 12 minutes before it tipped to 70 just at the end. It was my bad stating my issue was heat, its the sound the heat can produce due to fans, but I can live with that. I think I will stop here for now, should the urge present itself I may tweak voltages a little more, try reach 1300mhz core.
The 7950/7970 owners lounge on Overclock.net was actually where it was suggested I use MSI afterburner to increase the voltage to solve my issue with being unable to pass 1040mhz core clock in AMD overdrive. Great site though, it has solved many of my hardware related issues, I strongly recommend it.
No,you can overclock your cpu and ram,but this is best done in the bios. Or some MSI programs or even some motherboards give you overclocking tools,and this can be used to oc the cpu or ram, and oc-ing the cpu is allot more fun
Well then I look forward to this, cause OCing my gpu has been pretty fun. I don't look forward to the 10 hour stress tests at every point though

. I'll get into this once I get my replacement h100 back.