Good candidate for MISC too as anyone who's on the site came here initially for Trek. I say TNG - why? Because while s2 of TNG is shite, s3-7 are great. For ENT only s4 can be called great.
I'd say GTD is much better, but it's probably all good. Anyway, I picked the obvious answer (this coming from someone who likes Enterprise too). If you had posted it in The Neutral Zone, I would probably have voted the opposite way
Interesting choices....which for me would be roughly the equivalent of having to pick between "Fingernails on a Chalkboard" (ENT) and "Fingernails on a Politically Correct Chalkboard" (TNG). The REAL answer is TOS or DS9.
If you've never watched it TNG will look a bit dated to you. Depends on you if that bothers you or not.
That's like asking "Should I have steak or a bologna sandwhich?" TNG is way above and beyond Enterprise.