Welcome!
first things first, how long per day is the PC on? If its only on a few hours, you really need to be looking at the standard cpu client. It gives pretty poor points, but the deadlines are long and theres almost no risk of them not being completed! If your pc is on a good length of time per day (8hrs plus i think would be fine), the SMP client is the way to go. The windows SMP client is not officially supported as a service (or at least it wasnt when i had a go at running it), but im pretty sure it will run as one. It has the advantage of being multi threaded and is able to use all of the cores of a quad (albeit not hugely well). If you leave the pc on 24/7, you could try 2 SMP clients, although im pretty sure this is a little tricky, and is not how stanford would like you to run the client (their priority is getting the work units back ASAP... but this doesnt always get the most points!). Maximum ppd from the cpu will come from either a native linux install or from a couple of virtual machines running some flavour of linux, but these are not without their own disadvantages.
The GPU will crunch away endlessly without much effort/problems (at least in my experience). All you need for this is the current client, which i think is on the 'beta' page of the stanford client list still (its hugely stable despite this). There is a graphical client that minimises the client to the system tray when not open, which is quite convienient for stopping and starting, or a CMD window client depending on what your after. Im not sure about running this as a service, but the graphical client can be shut down by right clicking and selecting exit, or the CMD window based client simply by ctrl+c 'ing out of the window.
Also have a google for FahMon - a great tool for checking the clients.
FAH is pretty stressful on the system, but if you set all of the clients parametres to 'idle' you should be fine. If you run the SMP client, you need to set the gfx client to a slightly higher priority, else it will sit there doing nothing (there is an option for a 'low' setting in the client config). I use my pc for all sorts whilst running FAH - sometimes for films etc its better to manually change the priority of the media player to high using task manager to get smoother playback, but its not normally an issue. Its a similar story with the gpu client - with my 8800GT a few months ago, i set the client to use 80% of the gpu to make desktop + dvds smoother (again, a client config option), but i dont really need to do this on the new client with a GTX280. I think your milage may vary depending on setup/drivers etc, but i doubt you will have too many problems.
You may want to watch your overclocks, as FAH is pretty good at finding problems in this respect! Something like intel brun test/LinX gave me the best success for a folding OC (prime95 stable just wasnt stable enough).
Long post but i hope it helps! The initial setup is by far the hardest part, figuring out which clients/config is best suited to your machine/use of the PC. Its worth experimenting, but in the end everything helps. If you have any problems, people here are usually more than willing to help, and dont forget to post in the single machine crunchers list if your only using one machine!
EDIT: Appologies for the barrage of typos... i need to go to bed!
