>>54019556I can't really decide. I like them all for different reasons. And by 'all', I mean Gens 1 through 7.
Alola was the smallest region, but paired with the tropical island aesthetic, it was really comfy. Kanto and Johto lack any vareity with the limitations of the GB sprites, but the same limitations create its own aesthetic. It's uniform, and the music really paints a picture in your mind for different locations. Hoenn was the first to create memorable routes and locales with a variety of biomes. Sinnoh is probably the most bland. Unova really captured a lot of different architectural styles in both its towns and bridges, and sports the best applied soundtrack of the series. Kalos is quaint. It has a lot to look at, and a variety with it's different sections of the region.
I guess I don't really care for sinnoh. Especially when HGSS, of the same generation, had so much effort put into making it feel revived from the Gameboy monotony.
tl;dr - If I had to pick, I would probably say Alola nailed aesthetics, with perhaps Hoenn behind.