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Without doing any research:
2006 was the last game to emphasize the rivalry between Smackdown and Raw, the trailers and intro used Orton and Cena as the young figureheads for the war. 2006 Also had a bitchin story mode that elevated the series in that regard.
2007 introduced the interactive moves and had a demo showcasing this. It was the cross-platform iteration, I believe.
2009 was a personal fave of mine, and the last one I put serious time in. It enhanced a number of features of the series including create-a-move. It also had a pretty cool menu system. I see it as the first improvement on the series in a few years.
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