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Abstract Liquid crystal elastomers (LCE) are appealing candidates among active materials for 4D printing, due to their reversible, programmable and rapid actuation capabilities. Recent progress has been made on direct ink writing (DIW) or Digital Light Processing (DLP) to print LCEs with certain actuation. However, it remains a challenge to achieve complicated structures, such as spatial lattices with large actuation, due to the limitation of printing LCEs on the build platform or the previous layer. Herein, a novel method to 4D print freestanding LCEs on‐the‐fly by using laser‐assisted DIW with an actuation strain up to −40% is proposed. This process is further hybridized with the DLP method for optional structural or removable supports to create active 3D architectures in a one‐step additive process. Various objects, including hybrid active lattices, active tensegrity, an actuator with tunable stability, and 3D spatial LCE lattices, can be additively fabricated. The combination of DIW‐printed functionally freestanding LCEs with the DLP‐printed supporting structures thus provides new design freedom and fabrication capability for applications including soft robotics, smart structures, active metamaterials, and smart wearable devices. 

Abstract Mechanical metamaterials are architected manmade materials that allow for unique behaviors not observed in nature, making them promising candidates for a wide range of applications. Existing metamaterials lack tunability as their properties can only be changed to a limited extent after the fabrication. Herein, a new magneto‐mechanical metamaterial is presented that allows great tunability through a novel concept of deformation mode branching. The architecture of this new metamaterial employs an asymmetric joint design using hard‐magnetic soft active materials that permits two distinct actuation modes (bending and folding) under opposite‐direction magnetic fields. The subsequent application of mechanical compression leads to the deformation mode branching where the metamaterial architecture transforms into two distinctly different shapes, which exhibit very different deformations and enable great tunability in properties such as mechanical stiffness and acoustic bandgaps. Furthermore, this metamaterial design can be incorporated with magnetic shape memory polymers with global stiffness tunability, which also allows for the global shift of the acoustic behaviors. The combination of magnetic and mechanical actuations, as well as shape memory effects, impart wide tunable properties to a new paradigm of metamaterials.