The stick-slip phenomenon as a prevalent friction instability poses significant challenges to industry, including frictional vibration, reduced precision, and noise generation. The interfacial interactions between asperities on the surface of materials are critical in influencing stick-slip behavior. This study focused on modifying the asperities on the surface of zinc-coated steel through temper rolling as a new approach to suppress friction-induced stick-slip vibration and noise. It was revealed that temper rolling effectively suppressed the stick-slip behavior when the deformation of zinc-coated steel exceeded 2.3%. The proposed mechanism suggested that the temper rolling reduced surface asperity density, resulting in diminished potential energy fluctuations and a subsequent decrease in the stick-slip amplitude (the difference between the static and kinetic friction coefficients). In situ observation using the digital image correlation (DIC) technique demonstrated that the decrease in the stick-slip amplitude affected the motion state of the friction pair, effectively suppressing the stick-slip vibration and noise generation. These findings highlight the potential of temper rolling as an effective strategy for tailoring the surface topography to suppress the stick-slip phenomenon along with its related vibration and noise.