In this paper, we investigated the structure of SmCo films with different thickness and the effects of Cr buffer layer on the structure and morphology of SmCo/Cu thin films. Our data revealed that the degree of crystallization can be improved by prolonging the annealing time for thicker SmCo film. We also found that the surface roughness and the average grain size of SmCo can be decreased, as well as the intensity ratio (R) of SmCo(002) and Cu(111) reflection peaks be increased by adding Cr layer, consequently, the magnetic properties are enhanced. We concluded that the magnetic properties of SmCo/Cu films can be further optimized as varying the thickness of Cr buffer layers and increasing R values, in which, it is a crucial factor that the textile of Cu(111) and SmCo(002) was formed for SmCo/Cu alloy films.