Africa has been undergoing a rapid urbanization process, which is critical to the achievement of the 11th Sustainable Development Goal (SDG11). Using population density data from LandScan, we proposed a population density-based thresholding method to generate urban land and urban population data in Africa from 2001 to 2019, which were further applied to detect the spatiotemporal characteristics of Africa’s urbanization. The results showed that urban land and urban population have both grown rapidly in Africa, which increased by about 5.92% and 4.91%, respectively. The top three countries with the most intense urbanization process in Africa are Nigeria, the Democratic Republic of the Congo, and Ethiopia. The coupling relationship index of urban land expansion and population growth was 0.76 in Africa during 2001–2019. Meanwhile, the total proportion of uncoordinated development types at the provincial level was getting higher, which indicated an uncoordinated relationship between urban land expansion and population growth in Africa. Cropland, grassland, rural land, and forests were the most land-use types occupied by urban expansion. The proportion of cropland, grassland, and forests occupied was getting higher and higher from 2001 to 2019. The extensive urban land use may have an impact on the environmental and economic benefits brought by urbanization, which needs further research.