Using first-principles density functional theory combined with on-site Coulomb repulsion U, we have systematically studied the adsorption properties of transition metal (TM) atoms on strongly correlated NiO(001) surfaces with Fs centers (surface O vacancies). For the TM atoms, the adsorption on F-s centers is 1.26-3.18 eV more stable compared to positions near the surface O sites of defect-free NiO(001) surfaces. This indicates that F-s centers play an important role in the binding of TM atoms on O-defective NiO(001) surfaces. An analysis of the electronic structures and the charge redistribution for the adsorption of TM atoms on defective NiO(001) has been performed. The TM atoms are negatively charged, with charges ranging from -0.29 to -0.73 vertical bar e vertical bar. The TM-related states caused by interactions between TMs and surface defect states are found in the gap region of NiO. These results provide important information about controlling and understanding the adsorption properties of TM atoms on metal-supported ultrathin NiO films with surface defects like F-s centers. (C) 2015 Elsevier B.V. All rights reserved.