Mechanical properties, such as residual stress, micro-hardness and fatigue performance, of the Ti-5Al-4Mo-4Cr-2Sn-2Zr titanium alloy were improved via the laser peening without coating (LPwC) with a water-penetrable wavelength of 532 nm and pulse duration of 10 ns. In this paper, three kinds of laser energy, namely 85, 110 and 160 mJ were used to process the samples. The titanium alloy samples were also peened with different impact times (1, 3 or 5 impacts) at the energy of 85 mJ. The micro-hardness and residual stress distribution results provided that LPwC can introduce compressive residual stress (CRS) and also induce hardening of the target materials. Further, micro-hardness and CRS showed the increasing trends when the laser impact times increased. However, the CRS and micro-hardness decreased while the laser energy increased from 110 to 160 mJ, which was attributed to the dynamic equilibrium between the thermal and mechanical effects of LPwC. High cycle fatigue strength of the titanium alloy was significantly improved from 360 to 490.3 MPa after three impacts LPwC. The strengthening mechanism of fatigue strength subjected to LPwC was a combined effect between the laser-induced CRS and the high-density dislocations.