In this study, we demonstrate the synthesis of dynamic polysulfide networks through the solution poly condensation of pentaerythritol tetra(3-mercaptopropionate) (PTMP) with elemental sulfur by a reverse vulcanization process. Elemental sulfur content as high as 51% can be incorporated into the dynamic polysulfide networks. An important feature of the resulted polysulfide networks is their catalytic-free malleability, which implies that they have both thermo- and photo-induced solid-state plasticities to obtain a complex permanent shape due to the exchange of dynamic S-S bonds. These dynamic polysulfide networks have great potentials in fabricating complex three-dimensional shape memory devices for biological and mechanical applications.