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Adopting only a small amount ofazobenzene molecular to design liquid crystal photo-responsive materials capable ofquick response and flexible adjustability is in high demand but is challenging. Herein, azobenzenemolecules into polyurethane elastomer containing crystalline structure for preparing azobenzene liquid-crystal elastomers (ALCEs) are demonstrated and this phenomenon ofthe synergistic effects between liquid crystal and crystalline phase is discovered. The key point ofthe work is that the synthetic ALCEs can utilize the reversible isomerism capability of azobenzene molecules under light irradiation, which can pry the motion ofthe macromolecular crystalline region in system to realize the large macroscopic deformation ofthe photo-responsive behavior. Obviously, the ALCEs sample containing azobenzene molecule and polyethylene glycol crystallization can quickly bend, illuminated by ultraviolet light and rapidly straighten under green light. Under the same ultraviolet irradiation, the bending speed, final bending angle, recovery rate and recovery ratio ofALCEs are larger than that ofALCEs without any crystalline structure. This ALCEs based on the synergistic effects between liquid crystal and crystalline phase can break through the current dilemma that the application oftraditional azobenzene photo-responsive materials is limited by their concentration, greatly expanding the design thought and their scope ofapplication.