In the present work, TZ-3Y20A/Mo multilayer composites were prepared by sedimentation method. Appropriate settling parameters were chosen and green bodies of multilayer composites were obtained by settling TZ-3Y20A powder and Mo powder in turn according to the designed individual layer thickness. Then green laminates were hot pressed at 1773K for an hour under the pressure of 20MPa. Three-point Bending and Single Edge Notched Beam (SENB) tests were adopted to evaluate the flexure strength and fracture toughness of the samples. The results showed that, compared to TZ-3Y20A ceramics, the fracture toughness and the work of fracture increased due to the layered structure. The microstructure and crack deflection of the fracture surface of the laminated composites was also observed by optical microscopy.