The effects of surface modification on montmorillonite(MMT) were illustrated in order to produce the composite material with premium properties. MMT was treated with two coupling agents: glutaraldehyde(GA) and γ-methacryloxy-propyl-trimethoxy silane(KH570). The effects of different coupling agents on MMT and protein interaction were investigated by XRD, FT-IR, TGA, UV-Vis, etc. The results of structure characterization indicated that KH570 modification could change the surface crystal structure of MMT. However, GA reacted with amino groups of Bovine serum albumin(BSA) and the ordered layer structures of MMT were not completely destroyed. Coupling agents could greatly increase the amounts of BSA intercalated and the effect of KH570 is better than that of GA. And, the optimum concentrations of KH570 and GA were 2% and 6%, respectively. The rate of weight loss increased by about 12% after MMT was pretreated with coupling agents. The possible reason is that coupling agent treatment makes the structure of MMT more accessible to protein absorption and helps to stabilize the protein structure. Moreover,the presence of coupling agents can reduce the direct chemical interaction between BSA and MMT, which results in increasing protein desorption. The effects of surface modification on montmorillonite (MMT) were illustrated in order to produce the composite material with premium properties. MMT was treated with two coupling agents: glutaraldehyde (GA) and gamma-methacryloxy- propyl- trimethoxy silane (KH570) of different coupling agents on MMT and protein interaction were investigated by XRD, FT-IR, TGA, UV-Vis, etc. The results of structure characterization that that KH570 modification could change the surface crystal structure of MMT. However, GA reacted with amino groups of Bovine serum albumin (BSA) and the ordered layer structures of MMT were not completely destroyed. Coupling agents could greatly increase the amount of BSA intercalated and the effect of KH570 is better than that of GA. And, the optimum concentrations of KH570 and GA were 2% and 6% respectively. The rate of weight loss increased by about 12% after MMT was pretreated with coupling agents. The possible reason is that coupling agent treatment makes the structure of MMT more accessible to protein absorption and helps to stabilize the protein structure. Moreover, the presence of coupling agents can reduce the direct chemical interaction between BSA and MMT, which results in increasing protein desorption.