A gradient nanostructured surface layer of ∼600 μm in thickness was prepared on M50 steel with rare earth additions by a surface mechanical rolling treatment. The initial microstructure was refined into nanosized grains (∼29 nm in diameter) in the top surface layer, causing a significant increase of surface hardness. Meanwhile, the grain size increases, and the microhardness decreases gradually to the matrix values with increasing depth. Rolling contact fatigue tests showed that the fatigue lives are significantly increased by the gradient nanostructured surface layer. Analysis of failure mechanism revealed that both softening in the near surface layer and hardening in the subsurface occur under rolling contact testing. And surface spalling is the predominant failure mode, of which the cracks initiate from primary carbides in the top surface layer owing to surface softening. In gradient nanostructured samples, the nano-grains inhibit carbon migration by impeding dislocation movement in the near surface layer, so that martensite decay is suppressed. Consequently, the crack initiation is inhibited, and the fatigue property is enhanced.