Said it before and I'll say it again, I had the most fun with Arkham Knight and I think it's the best Batman game.
I honestly think City is retrospectively overrated. While I acknowledge the quantum leap in gameplay that it introduced, and it singlehandedly established the template for every Arkham game to come after, it's the game that I replay the least because I really don't enjoy the story. If they had just focused on the hook of a city-wide prison and Joker dying, I would have been fine. But the weird Protocol 10 subplot with Ra's and the underground Wonder City really detracts from the whole game, in my opinion. I will give City credit for having the best boss fight with Mr. Freeze and a memorable level with the Iceberg Lounge, though.
Arkham Knight by a wide margin. Combat and traversal were a huge leap over the previous games. On top of that, it took real advantage of its open world while still maintaining the strong interior game design that the series is known for; Stagg Airship and Panessa Studios were two great explorable hubs. Knight is just an excellent game all around and one of the best open world games ever made.
Arkham Knight is my favourite in the franchise. It is better on a technical scale, gameplay was dialled to 11, and the storytelling, I thought, was just fantastic. The side missions and other content just made for great replay value, in my opinion.
That said, Batman Arkham Origins is definitely the most memorable of the franchise for its intense story and remarkable boss fights.
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