For improving the vacuum and mitigating the electron clouds in ultra-high vacuum chamber systems of high-energy accelerators, the deposition of Ti-V-Hf-Zr getter film on a laser-treated aluminum alloy substrate was proposed and exploited for the first time in this study. The laser-treated aluminum surface exhibits a low secondary electron yield (SEY), which is even lower than 1 for some selected laser parameters. Non-evaporable getter (NEG) Ti-V-Hf-Zr film coatings were prepared using the direct current (DC) sputtering method. The surface morphology, surface roughness and composition of Ti-V-Hf-Zr getter films were characterized and analyzed. The maximum SEY of unactivated Ti-V-Hf-Zr getter film on laser-treated aluminum alloy substrates ranged from 1.10 to 1.48. The X-ray photoelectron spectroscopy (XPS) spectra demonstrate that the Ti-V-Hf-Zr coated laser-treated aluminum alloy could be partially activated after being heated at 100 and 150 °C, respectively, for 1 h in a vacuum and also used as a pump. The results were demonstrated initially and the potential application should be considered in future particle accelerators.