Rice (Oryza sativa L.) is one of the most important cereal crops in the world and a potentially important source of zinc (Zn) in the diet. The improvement of Zn content of rice is a global challenge with implications for both rice production and human health. The objective of the present study was to identify the effects of nitrogen (N) fertilizer rates and Zn application methods on Zn content of rice by evaluating rice production on native soils with different Zn availabilities in 2010/11. The results indicated that Zn application increased rice grain yield and Zn content in grains compared with the control; however, this effect was also affected by the native soil Zn availability, N fertilizer rate and Zn fertilizer application method. The native soil Zn status was the dominant factor influencing grain yield and grain Zn content in response to Zn fertilizer application. Grain Zn content ranged from 19.74 to 26.93 mg/kg under the different Zn statuses. The results also indicated that Zn application method has a significant influence on grain yield. Application of Zn fertilizer to the soil was more effective than the foliar spray on rice grain yield; however, the foliar spray resulted in a greater increase in grain Zn content when compared with soil application. Grain Zn content was affected by application method and displayed the following general trend: soil application + foliar spray > foliar spray > soil application. The experiments investigating the effect of N fertilizer rate combined with Zn application method showed a clear increase in both grain yield and Zn content as the N fertilizer level increased from 200 to 300 kg/ha. In addition, the results also indicated that N content and accumulation increased in all plant tissues, which suggests that Zn application might influence the uptake and translocation of N in rice plants. These results suggest that soil application in addition to a foliar spray of Zn should be considered as an important strategy to increase grain yield and grain Zn content of rice grown in soils with low background levels of Zn-associated diethylene triamine pentaacetate acid. Moreover, this process could be further strengthened by a high N application rate. In conclusion, these results demonstrate the potential of optimizing nutrient management using Zn fertilizer to obtain higher grain yields and higher grain Zn content in fields with low native Zn status.