From a technical standpoint (regarding graphics and gameplay features) Chaos Theory is the best, however I liked the missions in Pandora Tomorrow better.
All of them are great games that are worth playing. If you want to know with which one you should start I recommend starting with SC1, then SC:PT and then SC:CT. If you play them in reversed order you will most likely miss features of the newer games in the earlier games and the graphics get worse and worse. In my opinion that wouldn't do the games justice because they are all excellent. So if you start with the first one, you will like new features of the second and new features of the third one etc.etc.
So that's what I would do (and what I have done, although I played them all not too long after their release so I didn't do it intentionally).
Chaos Theory is a great game, but the Xbox 1 version of Double Agent is also worth a look; it has the best storyline in the series, looks just as good as Chaos Theory and uses the same gameplay engine, but I think the level design in Chaos Theory is a little bit better.
The first two that use the old gameplay engine are good too. Pandora Tomorrow being better than the first in my opinion because of it's more memorable and enjoyable level design. But neither are as good as the two later games on Xbox. So overall, Chaos Theory is my favourite.
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