Human activities have increasingly changed terrestrial particulate organic carbon (POC) export to the coastal ocean since the Industrial Age (19th century). However, the influence of human perturbations on the composition and flux of terrestrial biospheric and petrogenic POC sub-pools remains poorly constrained. Here, we examined 13C and 14C compositions of bulk POC and source-specific biomarkers (fatty acids, FA) from two nearshore sediment cores collected in the Pearl River-derived mudbelt, to determine the impacts of human perturbations of the Pearl River watershed on the burial of terrestrial POC in the coastal ocean over the last century. Our results show that although agricultural practices and deforestation during the 1930s–1950s increased C4 plant coverage in the watershed, the export fluxes of terrestrial biospheric and petrogenic POC remained rather unchanged; however, added perturbations since 1974, including increasing coal consumption, embankment and dam constructions caused massive export of both petrogenic POC and relatively fresh terrestrial biospheric POC from the river delta. Our data reveal that human activities substantially enhance the transfer of petrogenic POC and fresh biospheric POC to the coastal ocean after ca. 1974, with the latter process acting as an important sink for anthropogenic CO2.