Several polyarylates based on UV-sensitive bisbenzylidenoketones for use as potential second-order nonlinear optical (NLO) materials have been obtained by interfacial polycondensation. The polymers investigated can be divided into two groups: guest-host systems and polyarylates with NLO side-chains. The electro-optic (EO) coefficient, r(33), was measured in the Pockels experiment. UV crosslinking was applied to increase NLO stability of the investigated materials. Loss and time relaxation of EO coefficient for crosslinked and noncrosslinked polyarylates were also measured.