Biomaterials with the hydroxyapatite and biopolymers such as chitosan derived of crustaceans are is an alternative for bone repair. Carbon nanotubes have been a focus of interest because they can ameliorate the biomechanical properties of biomaterials. The objective of this study was to evaluate these materials in the repair of cranial defects in rats. The animals were divided in groups: without implant (G1), implanted with the chitosan/carbon nanotube membrane (G2), and chitosan/nanotube membrane mineralized with hydroxyapatite (G3). The animals were sacrificed 5 weeks after surgery and the skulls were removed for analysis of the defect area. The results showed absence of chronic inflammatory and little bone neoformation in the defect area of all groups. In G2 and G3 there was lack of reabsorption of the biomaterial that were encapsulated by connective tissue. In conclusion, the biomaterials were biocompatible, but their specific physicochemical properties did not indicate a considerable osteoregenerative capacity.