As I mentioned in the other thread: Blood Omen: Legacy of Kain is also great for that. The atmosphere in the game is a lot like Diablo 1, but more expanded. Diablo 1's atmosphere is very limited, as you're stuck with a dungeon and a town. Legacy of Kain takes place all over an entire country.
If you play it, you've basically got two choices. You can play the PSX version with ungodly load times, or you can play the PC version which has a fanpatch to add support for modern OSes and fix some bugs. There's a 3DO version(Indeed, I believe it was release same day as PC. PSX port happened later!) but I believe 3DO emulators still have issues, and finding a 3DO and a copy of the game is highly unlikely.
Edit: it also plays a lot like LTTP, but with a better combat system and, well, puzzles and such. It's one of the best Zelda games ever made.