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So, I'm still stuck deciding my Legion of choice.
Whichever Legion I choose will be Loyalist, so if it's a Traitor Legion, it's a loyalist element of the Legion. I like the aesthetic of each legion, and haven't really got a specific structure in mind for the army in question. Basically, I'm drawn towards Moritats and Legion Champions for my Centurions, breacher squads look cool. I'm mainly drawn to a good-all round army, leaning on elegance and close range power. So, thoughts?

From what you've said, Emperor's Children would probably suit you best. They believe they should be the best at everything.

I play loyalist EC myself, but given your comment regarding breacher squads, I voted for UM instead for you.
Legion Champions are certainly useful for EC, as it is a requirement to field the Maru Skara RoW.

Emperors' Children personally, you can use pretty much anything in the army and it would be fluffy, they have some amazing characters (Eidolon will destroy pretty much any non-Primarch, non-Sigismund character on the charge), their unique units are really fun to use and the play-style you are after of close range power and elegance pretty much sums up Emperors' Children to a tee.

If you like breachers then Ultramarines are great for that. They can go full Roman style as their breacher squads can swap boltguns for power swords, plus the Invictarii Suzerians which are quite nasty