Win against them (Brago & Sherry) in Story Mode.
To unlock the Create A Volcan mini-game, VS. Challenge Mode, and VS. Survival Mod, successfully complete the game.
First you need to achieve 100% in in your Zatch Collection. Then, press up, left, right, down, left, right, left, left, right, right during the title screen. If entered correctly,, the background will turn red. In story mode you should get item 27, the Glowing Red Book. You will also get a picture of the gang.