The synthesis of mesoporous silica/calcium phosphate composite loaded with the immunopotentiator tuberculin purified protein derivative (PPD-MS/CaP) as an effective adjuvant for cancer immunotherapy is reported here. The PPD-MS/CaP adjuvant is prepared by immersing mesoporous silica in a supersaturated calcium phosphate solution supplemented with the immunopotentiator PPD for 24 h. PPD is coprecipitated with calcium phosphate inside and on the surface of mesoporous silica. By loading the immunopotentiator PPD in the PPD-MS/CaP adjuvant, an enhanced activation of antigen-presenting cells, such as GM-CSF secretion by THP-1 differentiated macrophages, is obtained probably due to sustained PPD release and an efficient cellular uptake of PPD. The PPD-MS/CaP adjuvant mixed with liquid-N2-treated tumor tissue effectively triggers anti-tumor immune response and markedly inhibits in vivo tumor growth. The PPD-MS/CaP adjuvant is a promising alternative for cancer immune therapy.