Freeform Programmable Liquid Crystal Elastomers via Monolithic Integration of Co-Optimization and 4D-Printing
Liquid crystal elastomers (LCEs) are active materials capable of large, reversible thermally induced actuation, offering significant potential for applications such as artificial muscles and soft robotics. However, their broader deployment is hindered by the lack of a unified design-to-fabrication framework, the strong coupling among geometry, director fields, and manufacturing constraints, and the difficulty of reliably translating complex designs into physically realizable architectures. Here, we present an autonomous and monolithic integration of co-optimization and 4D printing that enables the end-to-end design-to-realization of versatile programmable LCE architectures with superior precision, complexity, and versatility. The proposed framework establishes a unified design strategy that co-optimizes the freeform multilayer geometry and fully continuous layer-specific director distributions, and subsequently translates the optimized fields into fabrication-ready DIW toolpaths through an automated manufacturing-aware pipeline. To bridge computation and realization, we develop an optimization-centered 4D printing approach with automated, fabrication-aware toolpath generation tailored for direct ink writing of LCEs. With the proposed design-to-fabrication paradigm, we experimentally realize architectures that exhibit complex, non-intuitive thermo-mechanical behaviors. Experiments achieve highly challenging prescribed functionalities beyond the reach of intuition-based approaches and show excellent agreement with numerical simulations across all samples. This work establishes a generalizable inverse design and physical realization of freeform programmable LCE systems, enabling function-oriented and optimization-driven intelligent LCE applications for next-generation soft robotic and responsive material engineering.