Liquid crystal elastomer (LCE) is a type of soft active material that generates large and reversible spontaneous deformations upon temperature changes, facilitating various environmentally responsive smart applications. Despite their success, most existing LCE metamaterials are designed in a forward fashion based on intuition and feature regular material patterns, which may hinder the reach of LCE’s full potential in producing complex and desired functionalities. Here, we develop a computational inverse design framework for discovering diverse sophisticated temperature-activated and -interactive nonlinear behaviors for LCE metamaterials in a fully controllable fashion. We generate intelligent LCE metamaterials with a wide range of switchable functionalities upon temperature changes. By sensing the environment, these metamaterials can realize maximized spontaneous area expansion/contraction, precisely programmable enclosed opening size change, and temperature-switchable nonlinear stress–strain relations and deformation modes. The optimized unit cells feature irregular LCE patterns and form complex and highly nonlinear mechanisms. The inverse design computational framework, optimized material patterns, and revealed underlying mechanisms fundamentally advance the design capacity of LCE metamaterials, benefiting environment-aware and -adaptive smart materials.

液晶弹性体（LCE）是一种软活性材料，可在温度变化时产生较大且可逆的自发变形，促进各种环境敏感的智能应用。尽管取得了成功，但大多数现有的 LCE 超材料都是基于直觉的前向时尚设计，并具有规则的材料图案，这可能会阻碍 LCE 充分发挥生产复杂和所需功能的潜力。在这里，我们开发了一个计算逆向设计框架，以完全可控的方式发现 LCE 超材料的各种复杂的温度激活和交互非线性行为。我们生产智能 LCE 超材料，在温度变化时具有多种可切换功能。通过感知环境，这些超材料可以实现最大化的自发面积膨胀/收缩、精确可编程的封闭开口尺寸变化以及温度可切换的非线性应力应变关系和变形模式。优化后的晶胞具有不规则的 LCE 模式，并形成复杂且高度非线性的机制。逆向设计计算框架、优化的材料模式和揭示的潜在机制从根本上提高了LCE超材料的设计能力，有利于环境感知和自适应智能材料。