A new technology, aluminizing after laser shock processing (LSP), for improving the fatigue performance of 1Cr11Ni2W2MoV-steel is advanced. The fatigue lives of samples are measured by the vibration fatigue experiment. These experimental tests show that the fatigue lives of aluminizing after LSP are greatly improved. The microstructures are examined by means of X-ray diffractometry (XRD), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The mechanism of fatigue life improvement is also discussed. Experimental results show that the thickness of aluminizing layer is found to increase because of this new technology, and the surface crystal of 1Cr11Ni2W2MoV-steel is distributed in a gradient manner.