It seemed more like he was only using her for his own objectives and he quickly discarded her when Mistress Nine was awakened and didn't care that she was killed. Even though she was a terrible person, I still felt sorry for Kaolinite and I think it would have made things interesting if he did actually love her and wasn't just using her.
I feel like between her wistful gazes at him and his obsessive laser focus fixation on creating a race of super humans, they probably haven't canoodled. It does seem that theirs is the most popular unrequited love thus far, though. I wish they could have been "healed" and then gotten married. Seeing good!Kaolinite as Hotaru's stepmother would have been interesting.
I've communicated in the past that I'm not that partial to shipping, and while I do have some ships I prefer, it's not a critical factor in my enjoyment to the series. However, I can't help but notice that quite a few of the ships I would have liked to have seen are of the unrequited pairings listed in the poll.
Before I get to the Other category, I will provide my thoughts on the couples I wish were canon.
Prince Demande and Neo Queen Serenity -- Let me stress the following. I would never want their existing canon equivalents to get together. I do not condone Demand's horrific acts in Sailor Moon media, and I'm not pretending what he did was right. However, I really wish a version of the two of them could have been a couple, if going by the old anime continuity.
One big factor is that in the old anime, between the dark energy and Wiseman's manipulation, we never did see much of what an uncorrupted Demande. Unlike the manga/Crystal where the self-styled Prince rebelled completely of his own free will, old anime Demande was clearly given a heavy push towards evil and cruelty. I'm not saying he wasn't a jerk as even Saphir's flashback indicated he was domineering, but it can never be known how much of the effect the Dark Crystal, negative energy, and Wiseman had on him. See the difference between the evil Spectre Sisters and the good Sepctre Sisters and even Saphir lost the mark of Black Moon Clan, proof that, yes, these people weren't entirely themselves. Conversely we also saw how evil Chibi-Usa became as Black Lady. Given that Demande did start to change his mind, there's some evidence he might not have been what we saw for the most of the time he was on screen. It's easy to read his desire for Neo-Queen Serenity as a twisted desire to want to change, or even worse, the subconscious knowledge that they would have been compatible under different circumstances..
Kaolinite and Professor Tomoe -- Again, this is more for the anime, since in the manga, both really are devoted to Pharaoh 90 in that version and neither is likely themselves. Like Demande, I don't think we really got to see what Kaolinite was fully like, as like nearly all the Death Busters, she had that pupilless gaze. Plus, it is somewhat cruel for her to serve Tomoe and Pharaoh 90, only for get killed for seemingly no reason. I would have loved it if not only she and Tomoe gotten together, but for Hotaru to have maybe a younger brother or sister.
Adonis/Danburite and Sailor Venus -- I wish this had been requited in either the past or the present. If it had been requited in the past, then it would have made Venus having to kill him a lot more tragic as they would have been meant to be if the Dark Kingdom didn't get in their way. If it had been requited in the present, then it would have shown the Dark Kingdom is no match for true love, and it would have given more hope that Mamoru could also have been brought from the brink.
Also, I would have liked for this to be requited because it would have been nice to see Venus in a romantic relationship (even her relationship with Kunzite in Crystal was backstory). I get the irony that Venus is a goddess of love but fails in romance, but I don't like it.
Makoto and Crane Game Joe -- Of all the one-shot crushes Mako had, this is the one I most of all wish were canon. There is so much about these two that make the perfect couple. She's a physical girl who is outgoing and fierce. He's an introverted, slightly cowardly guy with the power of telekinesis. She is a reincarnated warrior from the Silver Millennium, and he is a reincarnated warrior from the Dark Kinfdom. Plus, again Crane Game Joe was clearly being affected by Zoisite's first extraction attempt, so a lot of his less desirable actions could be chalked up (plus, I really don't see what was all that wrong with him running away from Mako and not "protecting" her; he's being targeted and he knows it, Mako is just collateral damage)
Makoto and Seijuro Ginga -- This was a one-episode crush, but it was one of Mako's better crushes, and I definitely prefer Jupiter and Ail as a couple to the love-square foolishness we got in the episodes. While, of course, this particular crush is boosted heavily by the old dub (where Alan did open up an become much more friendly to her), even in the original version, Ail did break his facade somewhat. Jupiter's theme is plants, woods, and trees, while Ail is a tree person, so thematically, they really go together. I even put together a fan screencap composition (old dub continuity, though, with Fiore as an Alan stunt double).
Seijuro Ginga/Ail and Usagi -- At the same time, of all of Usagi's various alternate love interests, I love this one the most. Ail was just right for her, in my opinion in a way that even Demande (who I support above) and Mamoru (who got away with a LOT of stunts). He doesn't love her for an ideal, because of a past life, or because she reminds him of a princess. He loves her because of her. To be fair, En's thought that he has done this before does undercut it, slightly, but it also supports the idea that Ail and En are really bad for each other (note how much more co-operative with humans -- even when they try NOT to be -- they are when separated and how much more malicious they get when they get together). Plus, unlike most of the unrequited ships, there are hints that if it weren't for Usagi's memories of Mamoru, she would reciprocate his affections. She needs to move on from her past as much as he does.
Rei/Sailor Mars and Mamoru - I love Rei and Yuichiro, so I wouldn't break up their sorta-pairing, but I really loved the dynamic Rei had with Mamoru, even though, much like with Natsumi, Mamoru was more putting up with her presence than actively courting her. It would have been nice if despite him remembering being in love with the Princess, that he realized he was in love with Rei now.