GPU and CPU are both on the "warm" side if you are still at stock clock speeds. Those temps are just past what I get on my E8400 at 4.13 GHz and my 4850 at 750/1050 overclocks when I stress test.
If you haven't yet, enable fan control for your video card and turn it up a little. The BIOS control on those cards is usually set really at low at startup and doesn't ramp up the fan speed until it gets near the 80 degree point and then it screams at you. Bumping it a little from the start goes a long way to keeping it cooler in the long run. Depending on the tools you use to manage your card (CCC or third party like ATI Tray Tools), you may have to enable overclocking first to gain access to clock control.
If your case has a side vent fan for the GPU, need to make sure it is in the best place for your GPU. Many reference designs vent the hot air out towards the back of the case, with the intake being in the middle/towards the front of the case. The side vent might be blowing cool air into the cards exhaust. If it's strong enough CFM, it could be reducing the efficiency of the cooler. Might need to take it off and mount it so it pulls are away from the GPU, or move it to intake air more towards the front if you can. Also, might want to pulll the card out and check for dust bunnies in side the fan intake. It doesn't take long for some of the vents to get clogged. I pull mine every other month and blow air backwards through the exhaust port and grab about a pea sized lint ball out of there. May not sound like much, but those vent holes are really small. A can of air could probly do it while still in the case, but I keep forgetting to grab a new can when I'm out...meh.
On that note, clean your CPU heatsink as well--if you can pull your fan off easily, you might see a big coating of lent under it, like a thick spiderweb. Run a q-tip across it and peel that gunk off of it.
My case (Thermaltake V9 Black) has a big mesh area where a 240MM low CFM fan was mounted. It got in the way of my new monster CPU heatsink, so it had to come off. I instead mounted a 120 MM High CFM fan (khaze yhuni) towards the front side on standoffs on the inside (it roared if I mounted it directly to the panel) to help feed fresh air to the GPU intake and also my RAM, and a low cfm 80mm (also on standoffs) lined up at the GPU's exhaust ports at the back to help pull that hot air out of the case. I can overclock/overvolt the piss out of it (760/1100) and it doesn't break 54 degrees--but I don't like stressing it that much, so I notched it back down.
As for the CPU, if you are running the stock cooler you should look into a replacement for it if you are overclocking. While you can get a moderate overclock with a stock HS/Fan--there are much better ones out there. I love my megahelems with a Khaze-yuni fan on it, but it's a beast and barely fits in my tower--but I'm able to clock my 3GHz to 4GHz and run prime all night and it doesn't get over 47 degrees celsius.
Idealy, you want a HS with heatpipes and a fan. You'll need to get in there and measure the clearances to make sure you can fit some of the better heatsinks in there. The key things to measure are height of your ram from the board and height of any other components within 5 inches or so of your CPU (in case the HS is wide, need to know if it will provide enough clearance above the CPU), distance from center of CPU to RAM and other high components/edges of the case/fan assemblies near the CPU (double it to figure how wide you can go with it), and finally distance from the top of the CPU SOCKET (not the board) to inside wall of the case or side fan assembly if it's in the way (take off about 1/2 a centimeter, or maybe 1/4 of an inch for wiggle room). You can pretty much count on sites giving the dimensions in metric, so you may need to convert the measurements. Here's a handy tool: http://mg-jewelry.com/mmtoinches.html
Frostytech.com does some really nice reviews on heatsinks and fans, and updates them regularly. They keep a top 5 list (actuallly, it's top 10) that breaks them down by AMD/Intel and other categories like noise and such. They also have a big monster list of everything they've reviewed over the last year or so, so you can even look up older ones to compare them as well. Here's a link to the current top5, from there you can link to the master lists and such: http://www.frostytech.com/top5heatsinks.cfm
The Prolimatech Megahelems was the grand-daddy of heatsinks when I got it. But most any of the ones that look like a tower of fins with heat pipes running through them generally all make a MAJOR difference in temps over the stock one. Because they use sealed vapor cooling, they don't have to be gigantic heatsinks to perform better than the stock, so you don't have to plunk down $100 bucks on one--some really nice ones can be found for socket 775 boards for under $50 depending on where you look. There's always ebay and newtech, but you can also find deals at places like crazypc.com, heatsinkfactory.com, and frozencpu.com as well. Scythe and Tuniq have some real good compact offerings that you can grab around the $40 mark. I think BestBuy is still carrying a compact universal Rocketfish one for like $30 that is a step up from stock even.