In recent years, the production of waste polyurethane and waste rubber has been on rise, and their resourceful recycling has become a research hotspot. In this paper, propylene glycol was used as alcohololytic agent to decompose polyurethane foam at different temperatures and polyurethane alcohololysis products were used as devulcanizing agent to realize the mechano-chemical reclamation of waste rubber. The polyurethane alcoholysis product at the lower layer (PAPL) contains more amine groups, which can combine with the free radicals generated during the rubber reclamation process to enhance the degree of devulcanization of rubber, thus improving the mechanical properties of the reclaimed rubbers (RRs). Compared with RRs filled with the activator only, the addition of PAPL can shorten the optimal vulcanization time of RRs and increase the crosslink density. The best overall performance of the vulcanized RRs is achieved using PAPL prepared at 180 ℃, with the tensile strength of 15.6 MPa and elongation at break of 325.5%. The method realizes the dual high-value recycling of waste polyurethane and waste rubber and shows promising prospects. This article provided a practical and feasible method for the dual high value utilization of waste polyurethane and rubber, and provided a new approach for the reuse of waste polyurethane products through chemical recovery.