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Severe surface hardening problems during laser surface texturing (LST) exert a remarkable influence on the tribological performance and fatigue strength of LST-treated components. Given this, an attempt is made to evaluate the effect of process parameters, including the energy density, the pulse frequency, and the scanning speed, on the hardness of laser surface textured 5A06 aluminum alloy based on response surface methodology. Firstly, a series of LST experiments were carried out by a nanosecond pulsed laser. Then, the predictive model correlating the process parameters with the hardness was established and tested for adequacy using analysis of variance. Sensitivity analysis was subsequently employed to identify and rank the significance of each process parameter. The results indicated that the developed model could effectively predict the hardness of laser surface textured 5A06 aluminum alloy. The scanning speed was found to be the dominant parameter, followed by the pulse frequency, and the energy density has the minimal influence. The graphical results revealed that the hardness gradually increases as the energy density and pulse frequency increases, while decreases as the scanning speed increases. This research could be used to select appropriate process parameters to manufacture high-performance surface textures with superior properties.