Toxic heavy metal containing Cr(VI) species is a serious threat for ecological environment and human beings. In this work, a new mussel-inspired polydopamine microsphere (PDA-sphere) is prepared through in situ oxidative polymerization at air condition with controllable sizes. The adsorption of Cr(VI) ions onto PDA-sphere is highly pH dependent with the optimal pH ranging from 2.5 to 3.8. A rapid Cr(VI) removal can approach in 8 min for equilibrium. More importantly, the prepared materials exhibit a remarkable sorption selectivity, coexisting SO42- NO3- and Cl- ions at high levels; The applicability model further proves its effective performances with treated capacity of 42,000 kg/kg sorbent, and the effluent can be reduced from 2000 ppb to below 50 ppb, which meets the drinking water criterions recommended by WHO. 1 kg sorbent can also purify approximately 100 t Cr(VI) contaminated wastewaters basing on the wastewater discharges of China. Such capacity for application ranks the top level for Cr(VI) removal. Additionally, the exhausted materials can be well regenerated by binary alkaline and salts mixtures. Such efficient adsorption can be ascribed to the well-dispersed morphology as well as the strong affinity between Cr(VI) and catechol or amine groups by XPS investigation. All the results suggest that polydopamine microspheres may be ideal materials for Cr(VI) treatment in waters. (C) 2017 Elsevier B.V. All rights reserved.