Developing recyclable adsorbents for co-capture of I2 and CH3I gas is a meaningful and challenging topic. Herein, Cu0-based mesoporous silica (C-S) materials were synthesized and applied for CH3I capture for the first time. Factors (Cu0 content, temperature, contact time and CH3I concentration) affecting the adsorption behavior were investigated. The results demonstrated that the CH3I adsorption capacity of the obtained C-S materials reached up to 1060 mg/g at 200 ℃. Furthermore, the C-S material exhibited excellent reusability (91.3 %, 5 cycles). It was found that Cu0 could cleave the carbon iodine bonds, causing CH3I to dissociate into •CH3 and I-. Then the Cu+ converted from Cu0 reacted with I- to achieve the purpose of CH3I capture. The adsorption mechanism of CH3I on the C-S materials could be concluded that Cu0 reacted with CH3I form CuI (Cu + CH3I → CuI + •CH3). This work suggested that the obtained C-S materials could be promising adsorbents for CH3I capture.