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Anisotropic CuCrO₂ thin films were successfully prepared on glass substrate by the electrospinning method followed by annealing at 600 °C. The directionality of the nanowires increased with increases in rotation speed. In addition, the structural formation and optoelectronic behavior of the CuCrO₂ thin films have been studied by X-ray powder diffraction studies, transmission electron microscopy, field emission scanning electron microscopy, and UV-vis spectroscopy. The X-ray diffraction studies revealed a delafossite properties of the CuCrO₂. The electrical conductivity in the parallel and vertical directions of the films produced at 2000–3000 rpm differed by two to three orders of magnitude. The optical transmittance properties of the CuCrO₂ thin films were improved by increasing the rotation speed.