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Naturally exposed rusted rebar has been widely used for the production of reinforced concrete. However, rusted rebar is prone to corrosion under chloride ion (Cl&minus, ) contamination and/or at a low alkalinity of concrete. This study employed two surface modification methods, sand blasting and wire brushing, to augment the corrosion resistance of naturally exposed rusted rebar. Electrochemical tests revealed that the surface-modified rebar displayed a significant improvement of passivation in the concrete alkaline environment and anticorrosion performance in both the Cl&minus, free and Cl&minus, containing simulated concrete pore solutions of different alkalinity. The enhanced performance was mainly due to the elimination of the rust layer and the direct exposure of the fresh metallic surface to the alkaline medium. Moreover, the effect of surface nanograins on the intensified passive film led to the best passivation performance of the wire-brushed rebar. The overall findings demonstrate that the two developed methods were conducive to the passivation and anticorrosion performance of the rusted rebar and thereby hold great promise for improving the service life of the reinforced concrete structures.