There's not many orchestrion rolls of music not in the game; the exceptions are the special arrangements you get as an order bonus for certain albums. The piano arrangements or Primals live performances of various songs, or the symphonic arrangements from the Eorzean Symphony albums. But in general, nearly every orchestrion roll of music is content from in the game.
Now, some of the orchestrions were of 1.x tracks or stuff from seasonal events, which didn't show up in game often, but they still were actual game-content music.
It's also worth noting there are actually very few true repeats on the mainline soundtracks; it's why if you want, say, "Steel Reason" (the Garlean 'boss fight' music still used even now) you actually have to get the 1.x soundtrack, 'cause I don't seem to recall it being on any later soundtrack, as it was never re-orchestrated. Similarly, Louisoix's theme, Canticle, is still used a lot in the game, but as it was never re-arranged for later content it's still only on the 1.x soundtrack.
There are places where a given song occurs a second time, mind you, but as implied by the above it's usually a re-orchestration or re-arrangement of the original used in some later bit of content, even if it's under the same title; witness Pitfire -- the amal'jaa theme -- which can be found on two separate albums, but as different arrangements. (The 1.x version and ARR versions are distinct different variations of the same work.)
And, confusingly, there are also a few places where you get different tracks with the same title. One of the bits of music for Titan EX is called Heartless, while the music for Alphascape v4.0 is also called Heartless, but is an entirely different piece. (And one of my favorites, as it works together a whole bunch of past musical themes -- and the franchise 'Prelude' leitmotif -- to evoke the Warrior of Light's entire journey up to that point.)
So, like Valkyrie said, if you want as many songs as possible (of actual in-game music) with as few repeats as possible, the answer is "buy the entire set of main game soundtracks, but skip the Primals albums, the piano albums, the Eorzean Symphony albums, Pulse, etc."
So:
- Before Meteor (1.x music)
- A Realm Reborn (2.0 music)
- Before the Fall (2.1-2.55 music)
- Heavensward (3.0 music)
- The Far Edge of Fate (3.1-3.56 music)
- Stormblood (4.0 music)
- Shadowbringers (4.1-5.0 music, oddly)
- Death Unto Dawn (5.1-5.55 music)
- Endwalker (6.0 music) -- only up for preorder right now.
Any other album you can safely skip as it'll be music not in the game (piano arrangements, Primals performances, the Eorzean Symphony performances), interim releases of a couple of tracks that will be on a later album, etc.



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