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ZnSnN2 has potential applications in photocatalysis and photovoltaics. However, the difficulty in preparing nondegenerate ZnSnN2 hinders its device application. Here, the preparation of low-electron-density nanocrystalline ZnSnN2 and its device application are demonstrated. Nanocrystalline ZnSnN2 was prepared with reactive sputtering. Nanocrystalline ZnSnN2 with an electron density of approximately 1017 cm−3 can be obtained after annealing at 300 °C. Nanocrystalline ZnSnN2 is found to form Schottky contact with Ag. Both the current I vs. voltage V curves and the capacitance C vs. voltage V curves of these samples follow the related theories of crystalline semiconductors due to the limited long-range order provided by the crystallites with sizes of 2–10 nm. The I−V curves together with the nonlinear C−2−V curves imply that there are interface states at the Ag-nanocrystalline ZnSnN2 interface. The application of nanocrystalline ZnSnN2 to heterojunction solar cells is also demonstrated. [ABSTRACT FROM AUTHOR]