Crystallographically aligned nanocrystalline films of the ferromagnetic spinel CuCr2Se4 were successfully synthesized and their structure and alignment were confirmed by X-ray diffraction and high-resolution transmission electron microscopy. The average size of the crystallites is about 200–250nm, and their (111) crystal planes are parallel to the film plane. A good match of the film’s electronic structure to that of bulk CuCr2Se4 is confirmed by transverse Kerr effect measurements. Four easy 〈111〉 axes are present in the films. One of these axes is oriented perpendicular and three others are oriented at an angle of 19.5° relative to the film plane. The magnetic properties of the films are determined by a competition between the out-of-plane magnetocrystalline anisotropy and the in-plane shape anisotropy. Magnetic measurements show that the dominating type of anisotropy switches from shape to magnetocrystalline anisotropy near 160K, which leads to a switch of the effective easy axis from inside the film plane at room temperature to perpendicular to the film plane as the temperature decreases. At last, a moderately large, negative value of the low-temperature magnetoresistance was observed for the first time in CuCr2Se4 films.