I have put coffee gounds down and watched chipmonks, squirrels, and rabbits romp over that bed with no hesitation so I doubt that they would have any deterent capabilties.
Coffee grounds will not significantly change your soils pH.

When I first started my compost pile, I read that coffee grounds would keep out foxes. I've seen a couple, but was more worried about local dogs that get free and run around.
Anyway, all coffee grounds go in my compost pile, and I've had no trouble with wildlife, and we've got racoons, opossums, etc. I built my compost bin out of chicken wire and a four plastic posts, an animal could get in it easily.
Not sure what the coffee grounds do other than disguise the smell of other things, but it's worked for me. No animals in compost pile!

Nothing deters squirrels other than solid fencing, as far as I know! I have raised beds that are completely covered on all sides, just because of the squirrels. If anyone knows otherwise, I'd love to hear how!

I think my biggest problem is gonna be chipmunks. I originally thought I had gophers, but now I know it's chipmunks. I had 12 yards of compost delivered about 10 days ago, and they already dug a network of tunnels in it. And I see 'em climbing on it every now and then. I don't think that's a good sign. Anyone know a good way to at least minimize the impending devastation? I can't afford to put in a fence with a roof. Electric fencing isn't allowed here, unless it's for "active farmland". And I don't think I could afford to put sheet metal all around it--which I hear does work cuz they can't climb it. Maybe if I planted a small, easily accessible garden just for them, they'd leave my other stuff alone? Anyone ever try that?