To improve the mechanical properties of glass fiber reinforced polyphenylene sulfide(PPS) composite laminate, the rigid composite laminate was prepared by thermo-compression lamination using the flexible glass fiber cloth and PPS nonwovens as reinforcement and matrix. Using the mechanical test, XRD, PLM and SEM, the effects of hot pressing temperature and time, content of glass fiber and silane coupling agents on the mechanical properties, crystallinity and microstructure of the composite laminates were explored. The results show that the tensile strength, flexural strength and notched impact strength of the composite laminate with 50wt% glass fiber cloth are 286.0 MPa, 175.0 MPa and 61.6 MPa, respectively, where the composite laminate is hot-pressed at a temperature of 320℃ for 30 min under a pressure of 30 MPa. It is found that using the silane coupling agent KH560 can significantly improve the mechanical properties of composite laminates. The flexural strength reaches to 394.9 MPa and the flexural modulus reaches to 23.6 GPa. Meanwhile, the inter laminar shear strength and notched impact strength are 16.4 MPa and 81.0 MPa, respectively. The mechanical properties of composite laminate have been greatly improved by optimizing the experimental conditions and using the silane coupling agent to treat the surface of glass fiber.