In this work, the effect of surface self-nanocrystallization on low-temperature gas carburizing for AISI316L austenitic stainless steel has been studied. The surface ultrasonic rolling processing (SURP) was used to prepare nanostructured surface layers, and then the un-SURP and SURP samples were treated by LTGC at 470 °C for 10 h, 20 h and 30 h. In order to analyze the effect of surface self-nanocrystallization on low-temperature gas carburizing, optical microscopy (OM), atomic force microscope (AFM), scanning electron probe micro-analyzer (EPMA) and nano-indentation analyzer were used. The results show depth of SURP-induced plastic deformation layer was about 330 μm. Meanwhile, the surface hardness and elastic modulus were increased but the surface roughness decreased obviously after SURP. After low-temperature gas carburizing, according to the results of the thickness, carbon concentration, nano-hardness and elastic modulus of the carburized layer, the conclusion is that surface self-nanocrystallization carried by SURP has a negative effect on the low-temperature gas carburizing for AISI316L austenitic stainless steel and with the increase of carburizing time, the greater the adverse effect on carburizing.