With the relationships aspect, I'd err on the side of keeping the canon couples together in order to stop the romance consuming whatever else the story might have to offer. Relationship issues are a good way of developing the characters who make that couple up but unless the story is really about a non-canon ship, it makes more sense to work with the couples the show already gave you. That being said, I've no idea what you intended to do with those couples so you might already have that stuff in mind.
Some suggestions I thought of/would like to see;
- If Katara and Sokka are both in the South Pole, struggling in relationships with a partner who has other, time consuming commitments (Aang and his Air Acolytes, Suki and her Kyoshi Warriors) it would be great to see the Water siblings supporting each other through that. They bicker a lot but Katara and Sokka do really love each other and any opportunity to show the more tender side of their relationship should be taken.
- With this presumably set after the Search, Ursa being back should be a huge part of Zuko's life, perhaps even to the detriment of him fixing his relationship with Mai. Like I said up top, not that Maiko should be broken for good, but if they did get back together that Mai might find the same old problems persisting (Zuko being a neglectful boyfriend, though no longer because of stresses over Yu Dao but now because of him wanting to catch up with Ursa) and it might take Ursa, as an outsider to their relationship but in the Palace enough to observe them, to get Zuko to buck up his ideas about how he considers Mai.
- Not sure what you have planned for Toph in Omashu (rematch against Bumi maybe?) but if she and Mai are wandering around wherever it might be cool for them to run into one another (though how exactly Mai ends up in the EK is your problem)
- Sort of unrelated, but I'd be interested in seeing Hakoda moving on with his life after the war, as Kya has been somewhat avenged, the SWT safe again and his children more or less indep
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