Crystalline silicon (c-Si) solar cells have dominated the photovoltaic industry for decades. However, due to high reflectivity and the presence of numerous types of surface contaminants, the solar cell only absorbs a limited amount of the incident solar radiation. To improve the efficiency of the solar cell, anti-reflection and self-cleaning coatings must be applied to the surface. The main objective of this work is to synthesize an amorphous carbon nitride CNx thin film as a novel dual-function anti-reflection coating (ARC) for c-Si solar cells. The CNx film was synthesized by the RF magnetron sputtering technique and characterized by different chemical, structural, and optical analysis techniques. The performance of CNx film was investigated via measuring the reflectance, photoelectric conversion efficiency, and external quantum efficiency. The minimum reflectance was 0.3% at 550 nm wavelength, and the external quantum efficiency achieved was more than 90% within the broad wavelength range. The open circuit voltage and short circuit current density that have been achieved are 578 mV and 33.85 mAcm−2, respectively. Finally, a photoelectric conversion efficiency of 13.05% was achieved with the coated c-Si solar cell in comparison with 5.52% for the uncoated c-Si solar cell. This study shows that CNx films have promising application potential as an efficient ARC for c-Si solar cells as compared to traditional ARC materials.