Silicone elastomers-based materials have been extensively involved in the field of biomedical devices, while their use is extremely restricted due to the poor surface lubricity and inherent hydrophobicity. This paper describes a novel strategy for generating a robust layered soft matter lubrication coating on the surface of the polydimethylsiloxane (PDMS) silicone elastomer, by entangling thick polyzwitterionic polyelectrolyte brush of poly (sulfobetaine methacrylate) (PSBMA) into the sub-surface of the initiator-embedded stiff hydrogel coating layer of P(AAm-co-AA-co-HEMA–Br)/Fe, to achieve a unified low friction and high load-bearing properties. Meanwhile, the stiff hydrogel layer with controllable thickness is covalently anchored on the surface of PDMS by adding iron powder to provide catalytic sites through surface catalytically initiated radical polymerization (SCIRP) method and provides high load-bearing capacity, while the topmost brush/hydrogel composite layer is highly effective for aqueous lubrication. Their synergy effects are capable of attaining low friction coefficient (COFs) under wide range of loaded condition in water environment with steel ball as sliding pair. Furthermore, the influence of mechanical modulus of the stiff hydrogel layer on the lubrication performance of layered coating is investigated, for which the COF is the lowest only when the modulus of the stiff hydrogel layer well matches the PDMS substrate. Surprisingly, the COF of the modified PDMS could remain low friction (COF < 0.05) stably after encountering 50,000 sliding cycles under 10 N load. Finally, the surface wear characterizations prove the robustness of the layered lubricating coating. This work provides a new route for engineering lubricious silicon elastomer with low friction, high load-bearing capacity, and considerable durability.