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Gen 5 games were the ones I came back to after the "pokemon are for children" years of grade school and I remember really liking some of the design even back then.
Emboar, Gigalith, Swoobat, Seismitoad, Whimsicott, Cofagrigus, Zoroark, Sawsbuck (Autumn), Jellicent, Galvantula, Chandelure, Haxorus, Golurk, Bisharp and Volcarona are all solid designs IMO.