Should I Divorce These Two?

The way I see it you have two ways to go, either you run with it and yes, divorce them. That in itself can be good for story purposes. The other option is to have them try and work on their marriage first. Have them go on a date, try to flirt, see if it helps - and if it doesn't, then divorce them. 

I have to admit that, if I feel sims should be together, I alter their attractions to suit. So if my sim is married to a brunette artist I make sure they are attracted to brunettes who like artsy stuff. Even then, though, they can get a strained relationship.

I have a young couple in my rotation who are both heavily into music and art, met as children and (I feel) were destined to be together. But when they went to the same uni they always seemed to be strained and mean with each other. I kept at it and now they seem fine and their relationship has developed into a close one. But they've only been dating so far and are not married yet. It helped to have them flirting, kissing etc quite regularly. 

Awww that is so sad! I had a married couple who divorced because Lovestruck gave them problems. I tried to make their relationship work, but they decided to divorce on their own, so I let them do that.

If Maxwell and Ayla were my sims I'd probably try to save their marriage at first, but if it didn't work out I'd let them divorce. Divorce made my sims' life more interesting. I wasn't interested in playing them anymore, but when they divorced I started to play them again.

Lovestruck also made my Fengs divorce. I would have wanted to keep them together, but their relationship just got so bad I couldn't do anything. I tried changing their attractions and sent them to therapy, but nothing worked and I didn't want to cheat their relationship better. They have a kid and they still live together, but I should probably move Lily or Victor out, because they keep fighting.

elliebreton​ I did with this when Maxwell was unattracted to Ayla. I sent them to cupids counselling and all Maxwell did in therapy was complain about her hair! In this save, I changed up Maxwell's clothes to suit Ayla's favourite clothing styles and colours and she still finds him unattractive.  I had a story planned where they were going to move to Del Sol Valley so they could be near their second eldest son George (living right next door!) I've already triggered this using the SimRealist mod. 

To be honest, i don't see them staying together for much longer. I'll proceed with the moving story and see how it goes but i'll be surprised if their marriage lasts past 2014!  

This is sad😔 Personally I would divorce since it seems you have tried fixing their turn ons/offs and they're still not attracted to the other, and that moodlet 😟 
Lovestruck has brought a lot of challenges for my couples too, they're happy one moment but suddenly one is yelling at the other and it really tanks their relationship. I end up having to constantly cheat their relationship to fix it 🥲 Their even at a high attraction. It's sad but honestly if they didn't have a high attraction/compatibility I would go for a divorce

Wonder if it is a glitch for Love struck, but I don't actually own it.

If you tried everything, and neither Sim is happy, maybe divorce the two. They may be attracted to another Sim later on, and even though it would be sad, they may be happy alone or with new spouses. It may give you new game play, and maybe more kids. 

When I look at everything else about their relationship -- soulmates, best friends, amazing compatibility -- it seems like they should make a good effort to stay together. Maybe the costume trunk would spice things up a little. Or a little getaway together. And then if it doesn't work, it just isn't meant to be. Good luck in whatever happens.