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We demonstrate a postgrowth in situ chlorine passivation method for suppressing surface-dominant transport in Si nanowires (SiNWs). This scheme helps avoid misorientations and meandering while facilitating the passivation of surface states. The leakage current of bridged SiNWs exhibited close to five orders of magnitude reduction as a result of chlorine passivation. The micro-Raman spectroscopy clearly reveals the nature of the varieties of silicon-chlorine bonds of the passivated devices. The chlorine-passivated SiNW surfaces are found to be stable over a long period of time with high immunity to environmental degradation. The chlorine passivation implies an effective and reliable method that can be tailored for mass manufacturing of nanowire-based devices.