LaserDisc is superior in many ways. It has almost double the resolution and can have analog or digital audio tracks. They can be comparable to early DVD releases. VHS is about half the resolution of a DVD and has analog (usually mono) audio tracks. S-VHS actually has a comparable resolution to LaserDisc, but releases such as this are just plain old VHS.
This Star Trek set does have Hi-Fi audio with Dolby B NR. What that means is if you're playing them on a Hi-Fi VCR (it will say "Hi-Fi somewhere on the front) you will get stereo audio and will sound a bit better than typical VHS. They will still work in a non-Hi-Fi VCR, but you will just have standard VHS mono audio.
As for how they look though, I might not be the best person to ask. I've watched a few of these tapes on an HDTV, and while they're far from HD quality I have no problem enjoying them. Watching VHS, to me, is kind of charming in a way. Or maybe it's just nostalgia. I think it also suites something like this show better. This is how I originally viewed the show. Old VHS tapes rented from the library or analog TV broadcast. So to me it looks just right. I have the series on DVD and BD. On BD they did a fantastic job remastering it, but I actually don't enjoy it as much. And in HD you can see when it's a stunt double a lot more often! I also love that the VHS tapes all have the trailer for the next episode after the end of each episode. I wish the DVD and BD had that.
But yeah, to be objective, if you're use to watching LaserDisc or DVD on an HDTV then VHS will be a noticeable drop in quality. I don't mind it, but you might. If you do get into VHS, definitely get a Hi-Fi player off eBay (some of them are not expensive) and clean the heads. Hi-Fi audio with cleaned heads will make a huge difference over a mono deck with dirty heads.
Interestingly, one of my favorite YouTube channels just posted a follow up video regarding upscaling VHS over HDMI. There's a lot of good info in them.
Original video:
https://www.youtube.com/watch?v=ZC5Zr3NC2PYFollowup:
https://www.youtube.com/watch?v=pQioCb4KUHM