The search for an effective zinc fertilizer and its application method to effectively increase zinc content and enhance aroma in rice grains is a crucial objective. In this study, a 2-year field plot experiment was conducted to investigate the influence of ZnO NPs foliar spraying on rice quality, grain zinc and aroma content, along with exploring the physiological mechanisms underlying these effects. Our results demonstrated that the rice breakdown value and taste value of foliar spraying zinc oxide nanoparticles were improved by 31.0-41.7% and 8.2-13.0% compared with CK (control treatment involved spraying water), improving the tasting and steaming quality of rice. While Fe and Cu content in grains decreased for the application of zinc oxide nanoparticles, zinc oxide nanoparticles foliar spraying significantly increased the zinc content and accumulation of grains by 33.6-65.1% and 37.8-74.7%, respectively. Further analysis showed that the sprayed zinc oxide nanoparticles achieved effective enrichment of zinc in edible parts and increased the final bioavailability of Zn. In addition, foliar spraying of zinc oxide nanoparticles significantly increased activities of nitrate reductase and glutamine synthetase in leaves, which elevated nitrogen content in leaves and grains, and ultimately enhanced 2-acetyl-1-pyrroline (2-AP) content in grains at maturity by 6.1-21.4% compared to CK. Our findings indicated that zinc oxide nanoparticles can be practically applied as a foliar fertilizer at the gestation for quality improvement, zinc enrichment and aroma enhancement of rice grains.