The spherical harmonic (SPHARM) description is a powerful surface modeling technique that can model arbitrarily shaped but simply connected 3D objects and has been used in many applications in medical imaging. Previous SPHARM techniques use the first order ellipsoid for establishing surface correspondence and aligning objects. However, this first order information may not be sufficient in many cases; a more general method for establishing surface correspondence would be to minimize the mean squared distance between two corresponding surfaces. In this paper, a new surface matching algorithm is proposed for 3D SPHARM models to achieve this goal. This algorithm employs a useful rotational property of spherical harmonic basis functions for a fast implementation. Applications of medical image analysis (e.g., spatio-temporal modeling of heart shape changes) are used to demonstrate this approach. Theoretical proofs and experimental results show that our approach is an accurate and flexible surface correspondence alignment method.