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Which regional dex best reflects the region's themes and aesthetic?
For me it's Hoenn. All the exotic animals and coloration go well with Hoenn's tropical and wild atmosphere. Afterwards probably Kanto, all the poison types and angry looking monsters combine well with the rough industrial shot hole that Kanto is. Afterwards, probably Sinnoh, a lot of fat Pokémon tell right away that the Pokémon have adapted to colder climates.
A tier below all of these I'd say Alola and Johto. Alola for the same reasons as Hoenn but it's significantly more tame and confy as a region, which is reflected in the designs. Johto's dex serves as an addendum to Kanto like the games were, they're subtle designs which demonstrates how hard they are to find and how they've managed to stay undiscovered for centuries.
At the end, I'd say Unova, Galar and Kalos. Unova's dex has a lot of cool mons individually, but I feel like it lacks an identity. It's blatantly aping Kanto which I guess fits well with Gen 5 being a soft reboot, but idk, something feels really off. Kalos doesn't have bad designs but they're also all over the place and few of them strike with Kalos' aesthetic. Same with Galar.