We develop smart polymeric materials which bear the combination of both dynamic non-covalent and dynamic covalent bonds, thus providing an additional and distinctive advantage for the development of smart polymeric materials that can be easily reshaped, reused, and broken down to the constituting parts. Our approach towards dynamic networks relies on the in-depth understanding of molecular properties of the materials. We primarily focus on (1) utilizing single chain polymeric nanoparticles (SCPNs) for application in reusable coating materials and (2) developing siloxane-based reprocessable and reshapeable transparent and high modulus dynamic covalent polymeric network.