(Na,K)NbO3 is a promising candidate for lead-free piezoelectric materials. (Na1-xKx)NbO3 films (x = 0.3–0.7) were epitaxially grown on a (100)SrTiO3 substrate via pulsed laser deposition. The effects of substrate temperature and oxygen pressure during deposition on the crystallinity of the films were examined: both parameters affected the mosaic spread of the crystallites and the formation of an impurity phase. In this study, the optimum conditions for the preparation of highly crystalline films were a substrate temperature of 800 °C and oxygen pressure of ∼60 Pa. The lattice constants parallel and perpendicular to the substrate surface responded differently to changes in x: the constant parallel to the surface increased with increasing x, while the constant perpendicular to the surface was maximized at x = 0.5. The difference in the dependence of the lattice constants could be explained by the elastic distortion of the lattice.