Robust and stiff polymeric materials usually rely on dense covalent crosslinking, which endows them with excellent properties such as high durability and outstanding thermal stability. However, because of the strong covalent bonds within the network, these polymeric materials are not easily degraded or recycled, giving rise to uncontrolled accumulation of end-of-life plastics in seawater or soil. Here, we present a general strategy to fabricate high-performance supramolecular polyelectrolyte plastics with environmentally ion-dissociable properties in a facile manner. By combining dynamic supramolecular hydrogen bonding and multiple electrostatic crosslinking with hydrophobic interactions, the resulting stable supramolecular polyelectrolyte plastic possesses a tensile strength of 93.6 ± 3.3 MPa and a Young's modulus of 2.3 ± 0.3 GPa, outperforming most of the commercial plastics. More importantly, the unique supramolecular dynamic network structures endow the polyelectrolyte plastics with excellent remoldability, good recyclability, and efficient dissociation in seawater and soil under ambient conditions. The simple fabrication strategy developed herein for robust sustainable polyelectrolyte plastics appears to be applicable to other bio-sourced and synthetic polyelectrolytes. This work provides a practical way for fabricating sustainable high-performance plastics by elegantly designing the supramolecular networks of polyelectrolytes.