The global urbanization rate is accelerating; however, data limitations have far prevented robust estimations of either global urban expansion or its effects on terrestrial net primary productivity (NPP). Here, using a high resolution dataset of global land use/cover (GlobeLand30), we show that global urban areas expanded by an average of 5694 km2 per year between 2000 and 2010. The rapid urban expansion in the past decade has in turn reduced global terrestrial NPP, with a net loss of 22.4 Tg Carbon per year (Tg C year−1). Although small compared to total terrestrial NPP and fossil fuel carbon emissions worldwide, the urbanization-induced decrease in NPP offset 30% of the climate-driven increase (73.6 Tg C year−1) over the same period. Our findings highlight the urgent need for global strategies to address urban expansion, enhance natural carbon sinks, and increase agricultural productivity.