“…Covalent network materials, such as thermosets, are indispensable for their superior durability and thermomechanical robustness but also cause ever-increasing concerns because of their chemically unrecyclable nature . Considerable research efforts have focused on improving the sustainability of polymer networks by replacing the permanent 3D cross-linked network structure with reversible bond connectivity. , As a result, a plethora of covalent chemistry platforms have been developed to prepare dynamic polymer networks, thereby introducing material reshaping, healing, and reprocessing capabilities. − Predominantly thermal activation of the embedded dynamic cross-links has been harvested to induce covalent bond rearrangement and reshuffling of the network structure. A fundamental limitation using thermal equilibrium reactions, however, is the inability to exclusively trigger either the bond forming or bond breaking process in an orthogonal manner. , Hence, complete de-cross-linking and depolymerization back into the initial building blocks requires demanding reaction conditions (e.g., high temperatures) and/or additional chemicals (e.g., solvolysis) to shift the dynamic equilibrium toward the completely debonded state. , …”