Honestly, do not care much for the Pre-Sequel, probably one of, if not my least favourite game in the entirety of the franchise. Still great that it's included in this collection and it's not a bad game by any means, it's more Borderlands, and more content never hurts.
Borderlands 2 however is an amazing game that has aged particularly well and continues to look fantastic due to the artistic direction taken. Whilst movement may feel more "modernized" and "fluid" in Borderlands 3, it lacks a compelling villain and the writing is rather shoddy. Borderlands 2 on the other hand, whilst not exactly great in the narrative department either, had a more compelling villain and far more memorable, on top of humour that for many, will likely have aged poorly but for me, continues to hit the spot just right. It's juvenile as expected, and silly, but I still enjoy it even today. Gun-play is still solid and responsive and sound design is good across the board.
NOTE : This doesn't include the latest piece of content that they released "Commander Lilith and the Fight for Sanctuary". This won't be a big issue for some, but it does raise the level cap and provide some extra content. The reason I'm putting this in here, is because it is no longer free, and you're expected to front up £11.99 for it which, honestly is a ridiculous price tag for what you truly get from said piece of DLC. If I recall, it was a hype-tool for Borderlands 3 at the time, but even so, that price tag is iffy, so I'd suggest catching it on sale.
Borderlands THC however is worth every penny even at full MSRP though, though it goes on sale often enough and is old enough to justify some patience.