Printing Liquid Crystal Elastomers On-the-Fly: Freestanding liquid crystal elastomers “on-the-fly” are fabricated by a hybrid 4D printing method using laser-assisted direct ink writing. This process is integrated with Digital Light Processing for printing optional structural or sacrificial materials to create active architectures, such as active tensegrities, loading-bearing actuators, and 3D liquid crystal lattices, in a one-step additive process. (Adv.Mater.2022, 34, 2204890). Contributors: Xirui Peng, Xiaohao Sun, H. Jerry Qi, Shuai Wu, Ruike Renee Zhao