Versatile Photoluminescence Polymers for Printed Transparent Self‐Healing Optical Devices

Abstract The development of comprehensive optical self‐healing polyurethane polymers for smart optical devices presents a significant challenge due to the trade‐off between intrinsic self‐healing capability and mechanical strength. This study focuses on the synthesis of versatile photoluminescence supramolecular polymers that integrate self‐healing ability, mechanical strength, and fluorescence responsiveness. The incorporation of hydrogen bonds and disulfide bonds into the dynamic hard domain results in the optimal polymer exhibiting impressive mechanical properties (strength, 27.0 MPa; toughness, 132.1 MJ m −3 ; elongation at break, 1450%), as well as a conspicuous self‐healing efficiency (surface scratches disappear within just 1 min). Furthermore, the transparent (transparency >97%) and colorless polymers demonstrate aggregation‐induced emission, characterized by intense cyan fluorescence that transitions to subdued blue fluorescence upon stretching under 365 nm irradiation. Proof‐of‐concept experiments demonstrate that screen‐printed fluorescent patterns, based on as‐prepared fluorescence ink associated with dual‐mode upconversion emission, are able to successfully encode fluorescence information, and can be integrated into the self‐healable 3D optical devices. The self‐healing optical devices designed with versatile polymers and featuring diversified patterns offer a promising direction for the advancement and application of future self‐healing materials.