Oh, no question about it! The Elder Scrolls IV: Oblivion has the most memorable game soundtrack for me, period. It's absolutely gorgeous and atmospheric, ethereal yet comforting.
The droning strings and peaceful piano of
Auriel's Ascension stirs my heart in ways I can't explain, bringing to memory all the beautiful moments when I'd just let my character sit or stand somewhere to take in the views. It particularly reminds me of when I'd just have my character jump to the roofs of Bliss in New Sheoth (in the Shivering Isles) and watch in awe as the night-time pink spore clouds gently drifted overhead.
Then, there's the ambient outro of
King and Country which reminds me of intentionally walking my horse around the valleys of the Nibenay Basin during the day, enjoying the gentle sunlight and sound of the leaves rustling in the wind.
Or maybe
All's Well, which conjures images of my character sitting inside an inn in Anvil, enjoying the (sometimes comedic) banter between the NPCs as the gorgeous harp and flute serenade my ears.
Oh, and there's also great combat music, such as
Defending the Gate which appropriately feels like the soundtrack to a fierce defense. Sure, it sometimes feels a little less than right when battling a low-end enemy but when you hear it in the more epic battles later on, well... in the words of Todd Howard, "it just works."
And of course, there's the absolutely amazing theme track,
Reign of the Septims. While Skyrim's menu music has something special going for it, this rendition of the TES theme is just too memorable for me. It really does feel like the music of the final days of the Septim Empire: full of glory and prosperity that's all precariously teetering on the brink of total destruction.
All of this game's incredible soundtrack comes together to solidify why Oblivion is a top 3 game for me. It just helped sell the world to me and thanks to it, all of my great memories of the game are always just one listen away.