All the Infinity Engine games are worth playing. Suggested playorder: Balder's Gate, Balder's Gate II, Planescape: Torment. If you still want more after that, play Icewind Dale and Icewind Dale II, but neither are essential to play.
Fallout 1 & 2 are both great and worth your time. Also somewhat similar in spirit to those games is Arcanum. It's very rough around the edges, but those who love it, adore it.
Gothic 1 & Gothic 2 are worth playing. I'd liken them to the souls games to a certain extent, open world with a very tough sense of progression. Combat is quite wonky, though.
I'd also recommend Darklands. It's not as popular or well-known, but it's a great, mostly open-ended RPG experience that comes the closes to playing a tabletop RPG, IMHO.
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