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The recent use of ZnO nanoparticles (NPs) in agriculture has gained significant traction. However, the understanding of crop safety and environmental risk posed by ZnO NP exposure remains limited. As a result, this study administered varying concentrations of ZnO NPs (0, 10, 50, 200, 500, and 800 mg kg−1) to potato plants to determine their effect on food and soil quality. The results showed that while the number of tubers decreased, ZnO NPs enhanced the potato tuber quality and commodity rate and significantly increased Zn concentrations within various tissues. X-ray diffraction analysis showed that ZnO NPs at 50 mg kg−1did not penetrate the potato plants. From a soil environment viewpoint, higher ZnO NP concentrations significantly changed the physical and chemical properties of the soil but not the dominant groups of soil microbial communities. However, noticeable shifts in the relative proportions of these communities occurred. This study is the first to explore the biofortification efficiency and possible environmental risks of ZnO NPs on potato plants, providing a theoretical basis for the safe application of ZnO NPs in agriculture.