To improve the epoxy bonding properties of polyphenylene sulfide (PPS) matrix composites, CK-MMT and K-BF were prepared by modifying montmorillonite (MMT) and basalt fiber (BF) with cetyl trimethyl ammonium bromide (CTAB) and 3-Glycidyloxypropyltrimethoxysilane (KH-560) as the modifiers. CK-MMT/BF/TPU/PPS composites were prepared by injection moulding. The surface properties of the composites were tested and characterized by scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS), etc. The epoxy bonding and mechanical properties were studied by combining the single-lap-joint tensile shear strength test and notched impact test. The results demonstrated the successful preparation of the modified MMT and BF. With the addition of CK-MMT and K-BF in different ratios, the surface roughness and the contents of polar groups of the composites increased, which could effectively improve the epoxy bonding properties of PPS matrix composites. When the additions of CK-MMT and K-BF were 10 and 25 wt%, respectively, the composites had the best overall properties. It demonstrated a single-lap-joint tensile shear strength was 7.56 MPa, representing a 220.34% increase over that of thermoplastic polyurethane/polyphenylene sulfide (TPU/PPS) and a 477.10% increase over that of pure PPS.