In order to increase the vibration life of Ti6Al4V titanium alloy, warm laser shock peening (WLSP) is used to improve the damping properties and thus decrease the vibration stress in this study. Firstly, the Ti6Al4V specimens are treated by WLSP at different treatment temperatures from 200 °C to 350 °C. Then the damping ratios of untreated and WLSPed samples are obtained by impact modal tests, and the improvement of damping properties generated byWLSP is analyzed by the microstructures in Ti6Al4V titanium alloy. Moreover, the finite element simulations are utilized to study the vibration amplitude and stress during the frequency response process. Finally, the vibration fatigue tests are carried out and the fatigue fracture morphology is observed by the scanning electron microscope. The results indicate that the damping ratios of WLSPed specimens increase with the increasing treatment temperatures. This is because elevated temperatures during WLSP can effectively increase the α phase colonies and the interphase boundaries, which can significantly increase the internal friction of materials. Moreover, due to the increasing material damping ratio, the displacement and stresses during vibration were both reduced greatly by 350 °C-WLSP, which can significantly decrease the fatigue crack growth rate and thus improve the vibration fatigue life of Ti6Al4V titanium alloy.