* The Sand Bird ride. You run around the Sand Bird, collecting Red Coins, while the Sand Bird wonderfully screeches like a hawk.
* In Pianta Village, after getting all red coins, and when you're on the gigantic palm tree, you grab a piece of "fluff" (a giant dandelion seed), then it flies all the way to a cloud that has the Shine out in the middle of the sky.
* Bowser Jr. managing to get Mario framed for polluting Isle Delfino; even though it was largely Bowser's idea, The Reveal of Shadow Mario's true identity really establishes how cunning Bowser Jr. can be when he puts his mind to stopping Mario.
* The first appearance of Mecha-Bowser, combined with the Crowning Music of Awesome and the fact that he actually breathes fire at the screen.
* Even though she failed miserably, Peach deserves points for trying to vouch for Mario's innocence in the game's opening.