In this study, laser surface treatment was applied to alter the surface texturing and chemical compositions of fused deposition modeling (FDM)-printed PEEK/CF samples to improve the deficiency of inert surface of PEEK as adherend substrate. The influence of IR-laser parameters including treatment gaps, single pulse energy and pulse widths on surface properties and shear bond strength were discussed. The results indicated that surface roughness was enhanced with decreasing treatment gap or increasing pulse energy, which reached the highest value of Ra = 32.44 μm at 0.4*0.4 mm 2 treatment gap and 300 mJ single pulse energy. By adjusting laser pulse width, surface wettability changed from hydrophobicity to hydrophilicity. After micro-second laser ablation, the texturing structure was changed and acted as mechanical interlocking effect, and therefore make the shear bond strengths improve from 3.28 to 6.42 MPa compared with the untreated groups. On the other hand, functional groups on substrate surface were activated after nano-second laser ablation, which contributes to an enhancement of shear bond strength through chemical interaction between adhesives and substrates. Therefore, our work highlights an efficient method of laser surface treatment on the adhesion property of FDM-printed substrates.