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The reason Mario looks mad in the Super Smash Bros. games is because he's trying to be serious (he's one of the OG Smashers! people look up to him!) but has absolutely no idea how to look like he's being serious so he just goes >:( mwad.
Mario: >:(
Somebody: Hey, can you tell me where the kitchen is?
Mario: :D Yes, hello, I can help!