The fiber-resin interface is an important component that significantly affects mechanical properties of composites. Random vibration-assisted vacuum processing (RVAVP), a new method to improve the adhesion of the fiber-resin interface, was presented. The effects of different curing processes on mechanical properties were comprehensively assessed by combining the fiber push-out test, finite element model simulation, cure monitoring approach, and short-beam three-point bending test, and the correlation between fiber volume fraction and mechanical properties was quantified by a facile thermogravimetric analysis-based methodology. The results revealed that application of random vibration during the curing process can promote the impregnation of resin into fibers and impede the growth of interface defects while improving mechanical properties at the same time. For this reason, the laminates produced by RVAVP exhibited the average interfacial shear strength of 78.02 MPa and the average interface fracture toughness of 51.7 J/m2, which is obtained a 48.26% and 90.77% improvement compared with the 0 MPa autoclave process. With the large observed increase in micro-mechanical properties, the average interlaminar shear strength of 93.91 MPa showed a slight reduction of 5.07% compared with the 0.6 MPa autoclave process. Meanwhile, the mechanical properties tended to be stable at the fiber volume fraction of 65.5%.