The transition metal dichalcogenide ZrS2 is an important semiconductor and should be a promising material in the optoelectronic field, however, its optoelectronic properties and applications have seldom been reported. In this paper, we synthesized single-crystalline ZrS2 nanobelts for interesting applications in solar cells. A facile and effective approach to fabricate ZrS2 nanobelt network-embedded solar cells was represented by forming Schottky junctions between the contacts of ZrS2 nanobelts and metal Auelectrodes. The solar cell devices showed a high short-circuit current Jsc of 21.8 mA cm−2 and a cell efficiency of 1.2%. The photovoltaic mechanism was discussed by constructing their energy band diagrams. Present results would be important for the field of transition-metal-dichalcogenidenanostructure optoelectronic applications.