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In this paper, we propose a novel surface matching algorithm for arbitrarily shaped but simply connected 3-D objects. The spherical harmonic (SPHARM) method is used to describe these 3-D objects, and a novel surface registration approach is presented. The proposed technique is applied to various applications of medical image analysis. The results are compared with those using the traditional method, in which the first-order ellipsoid is used for establishing surface correspondence and aligning objects. In these applications, our surface alignment method is demonstrated to be more accurate and flexible than the traditional approach. This is due in large part to the fact that a new surface parameterization is generated by a shortcut that employs a useful rotational property of spherical harmonic basis functions for a fast implementation. In order to achieve a suitable computational speed for practical applications, we propose a fast alignment algorithm that improves computational complexity of the new surface registration method from O(n3) to O(n2).