Fe1-xCux alloy films sputter-deposited on water-cooled substrates under Ar gas pressures, PAr=8.9 and 0.23 Pa, were investigated by scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction measurements. The SEM and TEM studies show that the alloy films made under PAr=8.9 Pa have a columnar structure with a grain size of about 20 nm, while those made under PAr=0.23 Pa have a fibrous structure with a grain size of about 10nm. The primary solid solutions of both bcc and fcc phases are extended in the Fe-rich and Cu-rich regions, respectively in contrast to no solid solution in the equilibrium phase diagram. In the Fe1-xCux alloys made under a high PAr, moreover, the single phase regions more widely extend and the oxide phase, CuFeO2, coexists.