In this article, nine groups of laminates were prepared according to the Taguchi L9(33) test array to study the influence of three process parameters, including molding pressure, molding temperature, and holding time on the performance of unidirectional carbon fiber/polyetheretherketone (CF/PEEK) laminates. A differential scanning calorimetry test was employed to select a reasonable process parameters range. The transverse tensile strength of the laminates was measured, and the fiber–matrix interfacial bonding behavior of the tested samples was analyzed by scanning electron microscopy. The results showed that the significance of factors to transverse tensile strength were molding temperature, holding time, and molding pressure in sequence. The optimal molding process parameters for CF/PEEK composite laminate were molding temperature of 400°C, molding pressure of 3 MPa, and holding time of 30 min. The optimization results were meaningful for the extension and application of thermoplastic composites.