Chiral, helical, nonlinear optical polybinaphthalenes were prepared by covalent bonding of chromophores to the backbone of polybinaphthalenes via a Mitsunobu reaction. This was achieved in a two-step reaction, with the formation of a precursor polymer by a Suzuki coupling reaction, which was afterwards functionalised with chromophores. It was tried to achieve a chiral ordering of the chromophores by attaching them to a chiral, helical polymer backbone. Poled films of the polymers were measured for their second-harmonic generation effect and showed nonresonant nonlinear susceptibilities (chi(zzz)((2))(0)) up to 10.6 pm/V. (C) 2003 Elsevier Science Ltd. All rights reserved.