In this study, we simulated pasture to Pinus radiata land-use change with the Generic Decomposition And Yield (G'DAY) ecosystem model to examine mechanisms responsible for the change in soil carbon (C) under pine. We parameterized the model for paired sites in New Zealand. Our simulations successfully reproduced empirical trends in ecosystem productivity and soil inorganic nitrogen (N), and modeled an increase in soil C and a small decline in soil N after 30 years under pine. We determined the mechanisms contributing to soil C change based on an established hypothesis that attributes increases in soil C storage to three main factors: increased ecosystem N inputs relative to outputs, increased C/N ratios in plant and soil, or a shift of N from plant to soil. The mechanisms we attributed to the simulated increase in soil C under pine were increased soil C inputs through tree litterfall, and an increase in the soil C/N ratio. In the first 7 years following pine establishment, a decline in soil C was simulated; this was matched by a decline in soil N. The simulated longer-term increase in soil C with afforestation by pine contrasts with results from published field studies, which show either a decline or no change in soil C under pine. The discrepancy between measured and simulated changes in soil C was attributed to the G'DAY model overestimating the transfer of litter C into the mineral soil.