Linear-dendritic block copolymer hosts were synthesized by end-functionalizing poly(methylmethacrylate) with dendrons that acted as hydrogen-bonding acceptors for nonlinear optical chromophores. Second harmonic generation experiments indicate that the d(33) coefficients and maximum chromophore loading are increased in linear-dendritic block copolymer hosts over comparable homopolymer hosts. Transmission electron microscopy shows 5-10 nm chromophore domains, confirming the effective spatial dispersion of the chromophores. (C) 2009 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 47: 5017-5026, 2009