O yes, Legacy of Kain is probably the best I've ever heard, ever. Playing the original is my yearly Halloween ritual when I don't go out - turn out all the lights, turn the volume up, pipe it through the stereo, and play all night. His laugh is so chilling...amagad, Simon Templeman.
Also, yes, Xenosaga is really, really good, too. Same with MGS.
Valkyrie Profile had some terrific voice acting, but some of it sucked, too, so I can't toss that out there
And one would certainly be remiss not to mention just about every NIS game, particularly Disgaea. Only the original Laharl and Etna FTMFW.