The intercalation compound Fe0.95PS3(MV)0.11 (MV is the methylviol ogen cation) has been prepared. Its crystal structure and magnetism have been in vestigated by x-ray diffraction (XRD), susceptibility measurements and Mssbaue r experiments. Its XRD pattern can be indexed in a monoclinic unit cell with a=0 .879nm, b=0.944?nm, c=1.070nm, β=114.76°. The distance between layers of this intercalation compound is increased by 0.33nm compared with that of FePS3. Th e data of susceptibility show that second-order magnetic phase transitions have occurred when the temperature changed from 300K down to 4.2K. A ferromagnetic ph ase transition occurred below TC=84K. An antiferromagnetic phase tran sition occurred below TN=26K. The results of Mssbauer spectra taken in the t emperatur e range of 12 to 300K indicate that there are three kinds of divalent ions with their high spin states, which imply a charge transfer from guest to the Fe—S e g antibonding orbitals of the FePS3 host lattice, and some ions have been re leased from the FePS3 host lattice and then some vacancies have been formed. T he ferromagnetism originates from a canting of the spins of Fe2+, whe reas the antiferromagnetism occurred when the canting of the spins of Fe2+ have been modified at the lowest temperatures.