Tough call.
Final Fantasy VI is my all-time favorite game, but the version on Steam is not great. It's got an incredible soundtrack and a fantastic cast of characters to go with the traditional turn-based Final Fantasy combat. The problem is, the Steam version redrew a lot of the characters and backgrounds and so the art styles don't match up.
9 Hours, 9 Persons, 9 Doors is my favorite with a Steam version that I can actually recommend. It's an incredibly well-written visual novel that doesn't have or need any sex scenes. If you hate the genre for feeling too "anime" or just think all visual novels are porn in disguise, this one will change your mind.
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The Fallout franchise, at least the new(er) ones. Up to the 3rd :P
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My two absolute favorites are not on Steam.
But my third favorite is (Skyrim)
I like being able to live a life that isn't mine. (Escapism)
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Minecraft & Diablo II
Both will be around for years due to strong modding communities.
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Fallout 3 and Fallout New Vegas, definitely. They hit so many notes with me. I love the retro-future, the first person exploration and the post-atomic setting which I personally greatly prefer over the zombie apocalypse that seems to be much more popular today. My taste runs more to science fiction than horror. Plus, the selection and the quality of mods available is superb.
Choosing one or the other is difficult. In regards to the base game I prefer Fallout 3, as I enjoy having both the large urban area of downtown DC and the more open area outside. I definitely missed the large city and underground tunnels when playing New Vegas. Also I like Three Dog's style, prefer the music selection on Galaxy News Radio, and was a bit disappointed with the main quest's choice of which faction to side with as I would rather have thrown my lot in with the Kings or the Boomers than any of the major factions.
But what brings New Vegas up for me is the mod selection. It's clear that many modders' skills had grown from their work in Fallout 3 to create bigger and better ones for New Vegas. I'm particularly partial to mods that add new locations and player homes and some of the ones for New Vegas are astonishing for their scope and creativity.
I've yet to move on to Fallout 4 but I'm certainly looking forward to it. I don't know if the settlement building has discouraged modders from creating the elaborate locations and homes. I'll have to look into that before making the plunge.
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Tomb Raider (2013), followed by the Batman Arkham franchise.
You asked why, so here is my review of TR2013 as an explanation:
http://steamcommunity.com/id/genkicoll/recommended/203160
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