Cs is a common radionuclide present in nuclear wastes and released from nuclear power plant accidents. It is hard to be removed from water with traditional technology. The current study aimed at developing of efficient cost-effective adsorbent for removing Cs with modified MCM-41 with specific functional groups -SH. Mesoporous material MCM-41 was selected due to its large surface area and tunable pore structure. Functional -SH groups were grafted into the pores of MCM-41 to enhance its capability of selective adsorption of Cs from multi-element (Co, Sr) water solution. The adsorption results showed that the maximum adsorption capacity was 29.24 mg/g. Both Langmuir and Freundlich models described the adsorption processes of Cs, indicating co-existence of both monolayer and multilayer adsorption in the surface and inner pores of the materials. TEM, FTIR, and Raman spectroscopy analyses indicated that -SH groups were successfully bounded into the pores of MCM-41. The present study approved the surface functional modified MCM-41 which might be a good alternative candidate for cleaning up of radionuclide Cs from nuclear power plant accidents and relevant nuclear accident events.