We report on the influence of cross-link density of azobenzene-containing liquid crystal polymer networks (azo-LCNs) on the thermomechanical properties and the laser-directed bending of cantilevers consisting of these materials. Cross-link density of azo-LCN was increased by adjusting the length of photocuring from 1 to 120 min. The storage modulus (E′), loss modulus (E′′), and glass transition temperature (Tg) of the azo-LCNs increase with cross-link density. Increasing the cross-link density of the polydomain azo-LCN reduces the magnitude of the bending angle of the cantilevers. The relationship between the thermomechanical and photomechanical properties of the polydomain azo-LCN reported here is further elucidated in the examination of laser-directed bending over a wide range of temperature. The temperature dependence of the equilibrium photodriven bending angle is shown to be strongly related to the temperature dependence of the storage modulus for a given azo-LCN sample. Normalizing the temperature d...