Nitrous oxide (N2O) is an influential greenhouse gas (GHG) and an unregulated ozone‐depleting substance. The extent to which N2O emissions from natural forest soils have been enhanced by high atmospheric nitrogen (N) deposition in China during past decades is unclear; however, assessing land‐related N2O emissions for 2060 national "carbon neutrality" goal is urgent. In this study, we proposed a "gray box" conceptual model and deduced a linear relationship between soil N2O emissions and N deposition on a large scale. On this basis, we created a "process‐augmented data‐driven" approach using which we combined experimental N addition data from 38 Chinese forests with N deposition observation data to estimate regional soil N2O emissions. We found that the N2O emission budget of eastern China forest soils averaged 0.24 ± 0.07 TgN yr−1 from 1996 to 2015; of this, ∼36% (0.087 TgN yr−1) was directly induced by N deposition. Soil N2O emission rates (RN2O) fluctuated slightly after 2006, and the RN2Os of different ecoregions were significantly different (p < 0.001). Soil factors and N‐deposition‐related factors dominated the spatial variation of RN2O. Our findings provide country‐specific and ecoregion‐specific emission factors for national GHG inventories in China. Our approach bridges the gap between site‐level experiments and demand for regional N2O emissions, and is applicable for estimating N2O emissions in other countries/regions. Meanwhile, more N addition experiments are needed to comprehensively understand N cycling processes and extend the predictive capability of the approach. Plain Language Summary: Nitrous oxide (N2O) is a greenhouse gas that is around 300 times more powerful than carbon dioxide. As many countries and regions are aiming to achieve zero net carbon emission ("carbon neutrality") by the mid‐21st century, we need to evaluate the emissions of nitrous oxide to build an accurate picture of the current situation. However, it is difficult to estimate the emission of N2O from natural soils because the spatial variation is high. Inspired by the linkage between elemental nitrogen (N) that enters an ecosystem and N that leaves the ecosystem, we proposed a conceptual model and deduced a linear relationship between N deposition and soil N2O emissions. On the basis, we used experimental N addition data from various sites to quantify the linear relationship. Then, the N2O emission and its variation was estimated with dynamic N deposition data. In eastern China forests where the N deposition rate is exceptionally high, around 0.24 million tons of N2O‐N was emitted annually from 1996 to 2015, around 36% of which was directly induced by N deposition. From another perspective, soil N2O emissions in this region are expected to decline owing to pollution control practices and decreasing N deposition. Key Points: Eastern China forest soils emitted 0.24 TgN2O‐N yr−1 from 1996 to 2015N deposition directly induced ∼36% of emitted N2O from eastern China forest soilsDirect contribution of N deposition to soil N2O emissions increased from tropical to boreal forests [ABSTRACT FROM AUTHOR]