In many forest ecosystems, nitrogen (N) deposition enhances plant uptake of carbon dioxide, thus reducing climate warming from fossil fuel emissions. Therefore, accurately modeling how forest carbon (C) sequestration responds to N deposition is critical for understanding how future changes in N availability will influence climate. Here, we use observations of forest C response to N inputs along N deposition gradients and at five temperate forest sites with fertilization experiments to test and improve a global biogeochemical model (CLM-CN 4.0). We show that the CLM-CN plant C growth response to N deposition was smaller than observed and the modeled response to N fertilization was larger than observed. A set of modifications to the CLMCN improved the correspondence between model predictions and observational data (1) by increasing the aboveground C storage in response to historical N deposition (1850–2004) from 14 to 34 kgC per additional kgN added through deposition and (2) by decreasing the aboveground net primary productivity response to N fertilization experiments from 91 to 57 gCm⁻² yr⁻¹. Modeled growth response to N deposition was most sensitive to altering the processes that control plant N uptake and the pathways of N loss. The response to N deposition also increased with a more closed N cycle (reduced N fixation and N gas loss) and decreased when prioritizing microbial over plant uptake of soil inorganic N. The net effect of all the modifications to the CLM-CN resulted in greater retention of N deposition and a greater role of synergy between N deposition and rising atmospheric CO₂ as a mechanism governing increases in temperate forest primary production over the 20th century. Overall, testing models with both the response to gradual increases in N inputs over decades (N deposition) and N pulse additions of N over multiple years (N fertilization) allows for greater understanding of the mechanisms governing C–N coupling.