Prepreg tack plays a crucial role in dominating the part quality during the automated fiber placement (AFP) process. This study aims to study the effect of process parameters on the tackiness between prepreg plies for two kinds of prepreg materials and find the optimal combination for high resultant tackiness. Moreover, the surface characteristics are utilized to evaluate the tackdetermining mechanism. For this proposal, a shear test method based on the theoretical model is first developed to measure the tackiness between prepreg plies. Thereafter, the influence of each process parameter including lay-up speed, compaction force, and material temperature on the tackiness is investigated and analyzed through the single-factor method. The results show that process parameters exhibit distinct impacts on the tackiness for two kinds of prepreg systems while the tackiness force of the EH918 prepreg is much lower than that of the M21C prepreg. It is because the resin layer on the surface of the EH918 prepreg is much thinner and even in comparison with that of the M21C prepreg. Finally, the response surface method is utilized to investigate the interaction among process parameters and find the optimal combination for high tackiness. It is shown that different prepreg materials present the distinct optimal combination for high resultant tackiness. These results are significant for controlling the tackiness of prepreg materials by tailoring process parameters to satisfy the specific manufacturing requirements.