To improve the bonding strength and electrical conductivity(σ) of cold-sprayed Al coatings on polyetheretherketone(PEEK) substrates, laser post-treatment was employed as an effective strengthening method without decomposition of the polymer substrates. Optical and electron microscopy observations were used to examine the microstructures and tensile fracture surfaces of the Al coatings fabricated with various laser powers. X-ray diffraction and electron backscatter diffraction were employed to investigate the phase composition and grain information of each coating. Hardness, pull-out adhesion, and electrical conductivity tests were performed to investigate the effect of laser power on the mechanical and physical properties of cold-sprayed Al coatings. The results revealed that despite the formation of several hundred micrometer-sized pores on the PEEK side, the porosity of the laser post-treated Al coatings significantly decreased, and the particle–particle interfaces were greatly healed with increasing laser power. The heat input induced large-scale recrystallization and significantly reduced the dislocation density in the samples. The XRD pattern revealed that no oxidation phase appeared following the laser treatment under the protection of Ar. The electrical conductivity and bonding strength of the Al coatings increased by up to 40 % and 167.4 %, respectively, after the laser post-treatment.