This work investigated adsorption of carbon dioxide on Shirasu‐based materials with various pretreatment procedures. A Shirasu‐based material pretreated via calcination procedure followed by treatment in aqueous ammonia solution adsorbed significantly high amount of carbon dioxide compared with pristine Shirasu‐based material and the Shirasu‐based material pretreated via only solution treatment in aqueous ammonia solution. The ability improved through addition of appropriate amount of water before the adsorption process of carbon dioxide, and exhibited comparative adsorption amount of carbon dioxide with high performance materials previously reported.