The authors have successfully performed femtosecond laser peening on a 2024 aluminum alloy without any sacrificial overlays. Laser pulses were directly irradiated to the surface of specimens in the air without water film as a plasma confinement medium during the peening treatment. The fatigue life was improved as much as 38 times in comparison with base material at a stress amplitude of 195 MPa. The fatigue strength of the peened specimen after 2 × 106 cycles was 58 MPa larger than that of the base material. The femtosecond laser peening process has a great potential to be applied in various fields where conventional peening methods cannot be used, as this process can be performed under ambient conditions without the use of a plasma confinement medium such as water or transparent materials.