Abstract: Taking poly(oxypropylene)-polyamines (POP) and cetyltrimethyl ammonium chloride(OTAC) as modifier, modified montmorillonite(POP-MMT and OTAC-MMT) was prepared via cation exchange. 4,4'-diamino diphenyl methane bismaleimide (MBMI), 3,3'-diallyl bisphenol A (BBA) and bisphenol-A diallyl ether (BBE) were used to synthesize MBMI-BBA-BBE matrix. POP-MMT/MBMI-BBA-BBE and OTAC-MMT/MBMI-BBA-BBE composites were prepared from MBMI-BBA-BBE, POP-MMT and OTAC-MMT by in-situ polymerization method, respectively.The results of FTIR spectra show that new groups have been introduced into the layers of two kinds of modified montmorillonite and organized successfully. The XRD result reveals that the interlayer spacing of POP-MMT and OTAC-MMT increases compared with sodium montmorillonite(Na-MMT). The SEM images display that the surface of composites is more rough, modified MMT disperses uniformly, crazing and microcrack appear and direct in different directions, and the composites exhibit ductile fracture. The test results of mechanical properties of composites show that the tendency of the bending strength and the impact strength of composites first increase and then decrease, which are higher than that of Na-MMT/MBMI-BBA-BBE and MBMI-BBA-BBE, the mechanical properties increase significantly, especially the effect of OTAC-MMT/MBMI-BBA-BBE is more obvious.