Forest ecosystems play an important role in regulating global temperatures through their capability to take up and store CO2 from the atmosphere, but the magnitude and sustainability of this carbon (C) sink is critically dependent on the availability of nutrients, particularly nitrogen (N). However, the extent to which the absolute amount of N or modifications in plant and soil C:N ratios controls long-term forest carbon sequestration (Cseq) remains uncertain. To assess this, we analyzed the results of 135 global field studies that investigated the dynamics of C and N availability during forest succession. The results showed that the accumulation of C and N in plant (including above- and below-ground vegetation) and litter pools decreased with forest age and approached an equilibrium value in the latter stages of stand development. Plant and litter C:N ratios increased during the first 10–20 years and remained relatively stable thereafter. The analysis further showed that the relative importance of a change in the total amount of N or modifications in the C:N ratio, to increases in Cseq, varied with forest age. Whilst the relative importance of a change in the total amount of N increased with forest age, the relative importance of a varied C:N stoichiometry decreased with forest age. Overall, a change in the total amount of N was the more important factor contributing to C storage during forest stand development and the C stored in vegetation dominated the total ecosystem C pool. These results show that ecosystem N availability is a key factor supporting long-term forest Cseq during forest succession. As most of the C is found in above-ground vegetation, this pool is particularly susceptible to abiotic or biotic factors and anthropogenically-related disturbances.