Neil’s output is consistently good-to-great from a sound stand point. He’s long been committed to capturing the best sound possible and it shows. So, it’s hard to go wrong whether you get originals, remasters, or new ones.
I’ll throw out a few: Everybody Knows This Is Nowhere (remastered), Tonight’s The Night (original/early first); Barn (new). When it comes to originals/firsts you’re always taking a chance even if it’s near mint. You just never know. But they can be incredibly good—if you clean them (the more the better).
If you like his stuff, then it’s definitely worth digging into his discography.