The aim of the last part of this general study is to analyze the influence of the interfacial properties and, more precisely, the adhesion energy, between carbon fibers and PEEK on the final performance of unidirectional composites. A set of mechanical properties, i.e. interlaminar shear strength, longitudinal tensile and compressive and transverse tensile properties, of different unidirectional laminates with the same content (60% by volume) of carbon fibers is determined. It is first shown that the interlaminar shear strength is constant, whatever the type of materials. Therefore, this test is not appropriate to characterize the strength of the fiber–matrix interface in PEEK‐based composites. On the contrary, in agreement with previous work on other systems, it appears that the ultimate properties (longitudinal tensile and compressive as well as transverse tensile strengths and strains) of the laminates increase with the interfacial adhesion energy, whereas the stiffness of these composites remains unaffected in all cases.