Abstract
The precise, reversible, and diffusionless shape-switching ability of organic ferroelastic crystals, while maintaining their structural integrity, positions them as promising materials for next-generation hybrid photonic devices. Herein, we present versatile bi-directional ferroelasticity and optical waveguide properties of three isomorphous, halogen-based, Schiff base organic crystals. These crystals exhibit sharp bending at multiple interfaces driven by molecular movement around the CH = N bond and subsequent 180° rotational twinning, offering controlled light path manipulation. The ferroelastic nature of these crystals allowed the construction of robust hybrid photonic structures, including Z-shaped configurations, closed-loop networks, and staircase-like hybrid optical waveguides. This study highlights the potential of shape-switchable organoferroelastic crystals as waveguides for applications in programmable photonic devices.