In this work, the effect of picosecond laser radiation on ablating carbon fiber-reinforced polymer (CFRP) composite surface to increase the adhesive bond strength was analyzed. The experiment was conducted using a picosecond laser of 3 W average power with 532 nm wavelength, working at the 20kHz frequency. Effect of process parameters (scanning speed, beam overlap, and number of passes) on surface treatment of CFRP was analyzed and optimized for maximum shear strength using response surface methodology (RSM). Single lap shear test was performed on adhesively bonded laser-treated specimens using the optimized process parameter (for maximum shear strength) and maximum roughness. Acoustic emission data was collected during the shear test to investigate and characterize the failure mechanism. The morphology of laser-treated surface and shear tested surface was explored using scanning electron microscopy (SEM) and white light interferometer (WLI).