external energy input (e.g., electricity, heat, light, and humidity) into mechanical work to realize versatile and complex motions, allowing for a range of applications including soft robotics, artificial muscles, medical applications, and sensors. [2] In this context, photoactuators are particularly attractive because light can provide remote and noncontact energy supply and spatiotemporal control over the actuation. [3] Recently, a number of materials based on liquid-crystalline polymers, hydrogels, and photoswitchable moieties-bearing polymers that can undergo large deformation and reversible shape change arising from photochemical or photothermal effect have been designed and utilized to fabricate photoactuators. [4] Among them, the actuators using near-infrared (NIR) light as a actuation source seem more promising especially for biological applications owing to the deeper light penetration through tissues and less damage to biomaterials, as compared to UV and visible (Vis) light. [5] Thus far, studies of soft photoactuators have mainly focused on liquid crystal elastomers (LCEs) and networks (LCNs). [6] Two approaches are usually utilized to fabricate such actuators by either mixing photothermal conversion agents (e.g., carbon nanotube, graphene, metal nanomaterials, and organic compounds or materials) with LCEs or incorporation of organic dyes into polymer chains. [7] As such, the photothermal-induced LC-isotropic phase transition can be achieved and consequently impart the actuators with diverse intriguing motions such as bending, twisting, oscillations, and crawling. [7c,8] In order to realize complex shape deformation and multifunctionality of the actuators, controlling the spatial configuration of the LCNs in the directionality and hierarchical orientation is usually needed. [9] Some systems successfully achieve complex shape morphing by a single-layer LCN film with special LC orientation controlling, and in some cases, bi-and multi-layer systems comprised of a responsive LCN and a passive material layer are employed for this purpose. [8c,10] It is noted that constructing a single-layer, single-component actuator with complex shape deformations is highly desirable, thus increasing their versatility and the range of applications. [11] Semicrystalline polymers (SCPs) represent an important class of shape memory polymers (SMPs). Because of the ease Light-driven soft actuators with adaptive shape changes, diverse geometric morphing, and reversible macroscopic movements have gained everincreasing interest owing to their diverse applications ranging from biomedical to aerospace devices. Herein, presented is a near-infrared (NIR) light-stimulated actuator based on cis-1,4 polybutadiene-polyethylene semicrystalline copolymer. In the system, a newly synthesized croconaine dye, 2,5-bis[(6-(11-carboxyundecanoate)hexyl-4-carboxylate-piperidylamino) thiophenyl]-croconium, serves as both an NIR absorbing agent and crosslinker. Taking advantage of easy processability, two-way shape memory, and photothermal eff...