A new single nanowire based nanosensor is demonstrated for illustrating its ultrahigh sensitivity for gas sensing. The device is composed of a single ZnO nanowire mounted on Pt electrodes with one end in Ohmic contact and the other end in Schottky contact. The Schottky contact functions as a "gate" that controls the current flowing through the entire system. By tuning the Schottky barrier height through the responsive variation of the surface chemisorbed gases and the amplification role played by the nanowire to Schottky barrier effect, an ultrahigh sensitivity of 32 000% was achieved using the Schottky contacted device operated in reverse bias mode at 275 °C for detection of 400 ppm CO, which is 4 orders of magnitude higher than that obtained using an Ohmic contact device under the same conditions. In addition, the response time and reset time have been shortened by a factor of 7. The methodology and principle illustrated in the paper present a new sensing mechanism that can be readily and extensively applied to other gas sensing systems. © 2009 American Chemical Society.