Liquid crystal elastomers (LCEs) are active soft matter‐based materials with strong stimulus responsiveness and reversible, large‐shape morphing capabilities. LCEs have demonstrated broad and growing applications in soft robotics, wearable devices, artificial muscles, and optical machines. The actuation intelligence and advanced functionality of LCEs depend on the smartness and properties of structures. In this review, we discuss recent advances in structure‐induced intelligence of LCEs, specifically the integration of structural properties with the alignment and processing of LCEs. The structural design principles for three categories consisting of common structures (film, fiber, and tubule), smart structures (origami, kirigami, mechanical metamaterial, topology, and topography), and complex structures (monolithic and integrated) are presented. Various alignment controls of LCEs, including mechanical, surface, field‐assisted, and shear alignment, are capable of inducing structural properties. The coupling and collaboration mechanisms of the LCE structures and the generated functions are discussed. The review concludes with perspectives on current challenges and emerging opportunities.