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Two kinds of nanocrystalline indium tin oxide (ITO) powders with different crystal structures-rhombohedral and cubic-were prepared using a coprecipitation process through the control of pH of a mixing solution and aging time after coprecipitation. The two powders have the same particle size of 15nm in diameter but different morphologies (spherical for rhombohedral and rectangular for cubic). The gaseous ethanol sensing characteristics of the sensors prepared by the two ITO powders were quite different. The sensitivity of rhombohedral ITO sensor was high compared to that of the cubic ITO sensor across all temperatures. The reason for this is explained through the viewpoint of the binding energy as shown in XPS measurement and the surface structure relating to the crystal structure.