We provide a detailed treatment of Weyl-Titchmarsh theory for half-lattice and full-lattice CMV operators and discuss their systems of orthonormal Laurent polynomials on the unit circle, spectral functions, variants of Weyl-Titchmarsh functions, and Green's functions. In particular, we discuss the corresponding spectral representations of half-lattice and full-lattice CMV operators. (C) 2005 Elsevier Inc. All rights reserved.