A Schottky barrier can be formed at the interface between a metal electrode and a semiconductor. The current passing through the metal-semiconductor contact is mainly controlled by the barrier height and barrier width. In conventional nanodevices, Schottky contacts are usually avoided in order to enhance the contribution made by the nanowires or nanotubes to the detected signal. We present a key idea of using the Schottky contact to achieve supersensitive and fast response nanowire-based nanosensors. We have illustrated this idea on several platforms: UV sensors, biosensors, and gas sensors. The gigantic enhancement in sensitivity of up to 5 orders of magnitude shows that an effective usage of the Schottky contact can be very beneficial to the sensitivity of nanosensors. © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.