The chapter discusses the optically-healable supramolecular polymers, focusing on the chemical and mechanical properties of these materials. Key findings include: 1. **Chemical Analysis**: The 1H NMR spectrum of the macromonomer 3 is provided, and TEM micrographs of different Zn-based metallo-supramolecular polymers (3-[Zn(Ntf2)2]0.9, 3-[Zn(Ntf2)2]0.8, and 3-[Zn(Ntf2)2]0.7) are presented. 2. **Mechanical Properties**: Modulated DSC traces show irreversible transitions at 193 °C for the starting material and various Zn-based polymers. Dynamic Mechanical Thermal Analysis (DMTA) traces of films with varying Zn²⁺ ratios (0.7 to 1.0) reveal changes in storage modulus, loss modulus, and tan δ. 3. **UV-Vis Spectroscopy**: UV-Vis absorption spectra of 3 and its Zn(NTf2)2 and La(Ntf2)3 complexes are analyzed, showing the titration curves and solid-state absorption spectra. 4. **Healing Experiments**: Unsuccessful attempts to heal 3-[Zn(Ntf2)2]0.7 films using light in the 400-500 nm wavelength range are described, with toughness values before and after exposure. 5. **Dark Regions in TEM Images**: Analysis of dark regions in TEM images of Zn(Ntf₂)₂-containing samples indicates the presence of an inorganic contaminant, as confirmed by EDS and EFTEM analysis. 6. **SAXS and Stress-Strain Data**: SAXS data analysis and stress-strain experiment results are provided, including toughness values and force-displacement data. These findings collectively highlight the structural and mechanical properties of the supramolecular polymers and their potential for optical healing applications.The chapter discusses the optically-healable supramolecular polymers, focusing on the chemical and mechanical properties of these materials. Key findings include: 1. **Chemical Analysis**: The 1H NMR spectrum of the macromonomer 3 is provided, and TEM micrographs of different Zn-based metallo-supramolecular polymers (3-[Zn(Ntf2)2]0.9, 3-[Zn(Ntf2)2]0.8, and 3-[Zn(Ntf2)2]0.7) are presented. 2. **Mechanical Properties**: Modulated DSC traces show irreversible transitions at 193 °C for the starting material and various Zn-based polymers. Dynamic Mechanical Thermal Analysis (DMTA) traces of films with varying Zn²⁺ ratios (0.7 to 1.0) reveal changes in storage modulus, loss modulus, and tan δ. 3. **UV-Vis Spectroscopy**: UV-Vis absorption spectra of 3 and its Zn(NTf2)2 and La(Ntf2)3 complexes are analyzed, showing the titration curves and solid-state absorption spectra. 4. **Healing Experiments**: Unsuccessful attempts to heal 3-[Zn(Ntf2)2]0.7 films using light in the 400-500 nm wavelength range are described, with toughness values before and after exposure. 5. **Dark Regions in TEM Images**: Analysis of dark regions in TEM images of Zn(Ntf₂)₂-containing samples indicates the presence of an inorganic contaminant, as confirmed by EDS and EFTEM analysis. 6. **SAXS and Stress-Strain Data**: SAXS data analysis and stress-strain experiment results are provided, including toughness values and force-displacement data. These findings collectively highlight the structural and mechanical properties of the supramolecular polymers and their potential for optical healing applications.