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Reasonable canopy structure and leaf physiological characteristics are considered as important factors for improving canopy nitrogen (N) distribution by matching the available light resources and thus increasing the grain yield of maize (Zea mays L.). However, the determinants of different maize varieties in light–N matching and grain yields with specific canopy structures and leaf physiological characteristics, as well as the response to the N application rate, remain poorly understood. In this study, we analyzed the relationships between different canopy structures and the enzyme activity and light utilization of spring maize in the field. Two maize varieties (XY335 and ZD958) with different canopy structures were used as the experimental material in a 2-year field experiment from 2014 to 2015, grown under different N inputs of 0, 100, 200, and 300 kg N ha−1 (N0, N1, N2, and N3) at a planting density of 90,000 plants ha−1 in Jilin Province on the Northeast China Plain. The results show that XY335 combined with N3 had a greater leaf angle, upper internode length and number, and upper leaf area index of the upper layer compared with ZD958. Higher N assimilatory enzyme (glutamine synthase (GS), glutamate synthase (GOGAT), and nitrate reductase (NR)) activities in the upper and middle leaves were observed in XY335 compared to ZD958. Furthermore, the light interception and light utilization efficiency of the upper leaves of XY335 increased, especially at higher N application rates, which significantly affected the N translocation post-silking and its distribution in different populations. As a result, the photosynthetic N use efficiency (PNUE) values of the upper leaves (10.4%) and middle leaves (5.2%) of XY335 were higher than those of ZD958, coordinating the canopy light and N distributions and being positively correlated with the maize grain yield. This suggested that the superior canopy structure of the upper layer and N assimilatory enzymes of the upper and middle leaves of this maize variety significantly increased the light interception of the canopy, while the synchronization of light and the N of the upper and middle leaves increased the light and N utilization efficiency of maize, which ultimately increased the grain yield at a high plant density. [ABSTRACT FROM AUTHOR]