Forest soils play a critical role in the sequestration of atmospheric CO2 and subsequent attenuation of global warming. The nature and properties of organic matter in soils have an influence on the sequestration of carbon. In this study, soils were collected from representative forestlands, including a subtropical evergreen broad-leaved forest (EBF), a coniferous forest (CF), a subalpine dwarf forest (DF), and alpine meadow (AM) along an elevation gradient on Wuyi Mountain, which is located in a subtropical area of southeastern China. These soil samples were analyzed in the laboratory to examine the distribution and speciation of organic carbon (OC) within different size fractions of water-stable soil aggregates, and subsequently to determine effects on carbon sequestration. Soil aggregation rate increased with increasing elevation. Soil aggregation rate, rather than soil temperature, moisture or clay content, showed the strongest correlation with OC in bulk soil, indicating soil structure was the critical factor in carbon sequestration of Wuyi Mountain. The content of coarse particulate organic matter fraction, rather than the silt and clay particles, represented OC stock in bulk soil and different soil aggregate fractions. With increasing soil aggregation rate, more carbon was accumulated within the macroaggregates, particularly within the coarse particulate organic matter fraction (250-2000 μm), rather than within the microaggregates (53-250μm) or silt and clay particles (< 53μm). In consideration of the high instability of macroaggregates and the liability of SOC within them, further research is needed to verify whether highly-aggregated soils at higher altitudes are more likely to lose SOC under warmer conditions.