The atomic structure of AIN/Al2O3 interface fabricated by pulsed laser deposition is characterized by high-resolution transmission electron microscopy (HRTEM) combined with systematic multi-slice HRTEM image simulations. It is found that the AIN film deposited on a (0001) Al2O3 substrate grows epitaxially with the orientation relationship of (0001)AIN//(0001) Al2O3 and [1100]AIN//[1120]Al2O3, with an atomically sharp interface. The observed interface showed best correspondence with the rigid structural model that AIN is terminated by Al at the interface, while the Al2O3 substrate is terminated by O. Detailed structural analysis indicates that Al sites at the interface are coordinated by both oxygen and nitrogen in this model, with similar coordination environment in AIN. This favored coordination state at the interface may stabilize the AIN/Al2O3 interface. (c) 2006 Springer Science + Business Media, Inc.