Across southern China, Moso bamboo has been encroaching on most neighboring secondary broad-leaved forests and/or coniferous plantations, leading to the land cover changes that alter abiotic and biotic conditions. Little is known about how this conversion alters soil carbon (C) and nitrogen (N). We selected three sites, each with three plots arrayed along the bamboo encroachment pathway: moso bamboo forest (BF); transition zone, mixed forest plots (MF); and broad-leaved forest (BLF), and examined how bamboo encroachment affects soil organic C (SOC), soil total N, microbial biomass C (MBC), microbial biomass N (MBN), water-soluble organic C (WSOC), and water-soluble organic N (WSON) in three forests. Over nine years, moso bamboo encroachment leads to a decrease in SOC and total soil N, an increase in MBC and WSOC, and a decrease in MBN and WSON. Changes in soil C and N occurred mainly in the topsoil. We conclude that moso bamboo encroachment on broadleaved forest not only substantially altered soil C and N pools, but also changed the distribution pattern of C and N in the studied forest soils. Continued bamboo encroachment into evergreen broadleaved forests seems likely to lead to net CO2 emissions to the atmosphere as ecosystem C stocks decline.