A polymer
nanoparticle network using single-chain nanoparticles
(SCNPs) as cross-links is designed. The experimental and theoretical
study shows that incorporating SCNPs in polymer networks leads to
smaller mesh size, faster terminal relaxation time, and reduced fluctuation
among cross-links, resulting in a significant increase in shear storage
modulus, and enhancement in tensile stress. Notably, the reversible
single-chain collapse of SCNPs under thermal stimulation enables the
polymer network to undergo coherent changes between two topological
states, thereby exhibiting reversible transformations between soft
and stiff states. This approach and finding can effectively tailor
the mechanical properties of polymer networks, potentially leading
to the development of intelligent, responsive materials.