Atmospheric nitrogen deposition may indirectly affect ecosystems through deposition-induced changes in the rates of insect herbivory. Plant nitrogen (N) status can affect the consumption rates and population dynamics of herbivorous insects, but the extent to which N deposition-induced changes in herbivory might lead to changes in ecosystem-level carbon (C) and N dynamics is unknown. We created three insect herbivory functions based on empirical responses of insect consumption and population dynamics to changes in foliar N and implemented them into the CENTURY model. We modeled the responses of C and N storage patterns and flux rates to N deposition and insect herbivory in an herbaceous system. Results from the model indicate that N deposition caused a strong increase in plant production, decreased plant C : N ratios, increased soil organic C (SOC), and enhanced rates of N mineralization. In contrast, herbivory decreased both vegetative and SOC storage and depressed N mineralization rates. The results suggest that herbivory plays a particularly important role in affecting ecosystem processes by regulating the threshold value of N deposition at which ecosystem C storage saturates; C storage saturated at lower rates of N deposition with increasing intensity of herbivory. Differences in the results among the modeled insect herbivory functions suggests that distinct physiological and population response of insect herbivores can have a large impact on ecosystem processes. Including the effects of herbivory in ecosystem studies, particularly in systems where rates of herbivory are high and linked to plant C : N, will be important in generating accurate predictions of the effects of atmospheric N deposition on ecosystem C and N dynamics.