Book of Vile Darkness, with Masters of the Wild close behind. Most of my books have seen some use, but the problem is that I have too many supplements and not enough game!
Right now, my answer to the original question would be RttToEE for the same reason Numion mentioned. However, ask me again a year from now and I strongly suspect the answer will be Savage Species.
The Banewarrens tops the list (I used it every week for about 8 months), right behind that would have to be the BoEM series, BoVD, Magic of Faerun (I also use FRCS quite a bit, it'd probably make the list)