Human activities have increased the imbalance in atmospheric N and P deposition, which changes soil nutrient availability and subsequently affects the structure and function of terrestrial ecosystems. Dioecious plants are important parts of terrestrial ecosystems and are characterized by sex-related differences in their response to the external environment and always exhibit a skewed sex ratio, which makes them more vulnerable to climate change and increases their risk of extinction. However, little attention has been paid to the effects of unbalanced N and P deposition on these plants, especially on their defense traits. In this study, we used dioecious Populus cathayana to investigate the influence of gradient N and P deposition on the correlation between growth and defense traits. The results showed that although the different rates of N and P deposition enhanced biomass accumulation in both sexes to varying degrees, the most substantial biomass increment was noted under a lower-nitrogen and higher-phosphorus (LNHP) treatment regimen, with females showing an approximately 112% increase and males a 47% increase in total biomass. In response to varying levels of simulated N and P deposition, males and females adopt distinct strategies for biomass allocation. Although declines in root biomass were observed in both sexes as nutrient availability increased, the decrement was more marked in males; under the LNHP treatment, it dropped by about 11%, while under a high-nitrogen and high-phosphorus (HNHP) treatment, the decrease was about 35%. Conversely, females demonstrated a heightened propensity to allocate biomass towards leaf development. Furthermore, with increasing N and P deposition, there was a general reduction in the concentrations of physical and chemical defense substances within the leaves of both sexes. Nonetheless, the correlations between defense substances, nutrient element content, non-structural carbohydrate (NSC) content, and dry biomass were more pronounced in males, suggesting a greater sensitivity to defense substance responses in males than in females. Overall, these results indicate that there is sexual dimorphism in the accumulation of chemical substances in male and female P. cathayana under unbalanced N and P deposition and they provide a technical and theoretical basis for predicting the population dynamics of dioecious plants, maintaining the stability of poplar populations, and constructing high-productivity poplar plantations globally in the future.