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Plasma spraying and magnetron sputtering were used to form graphite–copper films on an n-type silicon surface. The main objective of this work was to compare the properties of the obtained graphite–copper Schottky photodiodes prepared using two different layer formation methods and to evaluate the influence of copper content on the surface morphology, phase structure, and photovoltaic characteristics of the graphite–copper films. Surface morphology analysis shows that the surface of the formed layers using either plasma spraying technology or the magnetron sputtering method consists of various sphere-shaped microstructures. The X-ray diffraction measurements demonstrated that the graphite–copper coatings formed by plasma spraying were crystalline phase. Meanwhile, the films deposited by magnetron sputtering were amorphous when the copper concentration was up to 9.7 at.%. The increase in copper content in the films led to the formation of Cu crystalline phase. Schottky diodes formed using magnetron sputtering technology had a maximum current density of 220 mA/cm2 at 5 V. Meanwhile, the maximum electric current density of Schottky photodiodes formed using plasma spraying reached 3.8 mA/cm2. It was demonstrated that the efficiency of Schottky diodes formed using magnetron sputtering was up to 60 times higher than Schottky diodes formed using plasma spraying.