Rapid, Robust, and Reversible Photomechanical Bending in a Flexible Zinc(II) Complex Crystal with 2D Elasticity for Controlled Motion

The integration of rapid, reversible photomechanical responsiveness and 2D elasticity within a single coordination crystal remains a formidable challenge. Here, we report a Zn(II) coordination complex, [Zn(NCS) 2 (Z‐fppan) 2 ] ( Z‐1 , Z‐fppan = (Z)‐2‐(3‐fluorophenyl)‐3‐(pyridin‐4‐yl)acrylonitrile), where the synergy between photochemical isomerization and photothermal‐induced temperature gradients enables millisecond‐scale response. Driven by this dual mechanism, the crystal demonstrates robust and reversible photoinduced bending (>100 cycles). The generation of these localized stress gradients enables precise control over diverse photoactuated motions, including bending, rolling, and deflection. Additionally, single crystals of Z‐1 exhibit remarkable two‐dimensional elastic flexibility under mechanical stress, deforming reversibly along the (110)/(‐1‐10) and (‐110)/(1‐10) planes. The combination of rapid photomechanical actuation and mechanical adaptability presents a unique example of dual‐stimulus responsive behavior in metal‐organic systems. To demonstrate this practical utility, we leveraged this photomechanical behavior for wireless manipulation, successfully achieving remote‐controlled actuation. Such properties position Z‐1 as a promising candidate for light‐driven smart actuators and soft robotics.