Polyurethane (PU) is the 6th most produced plastic on a global basis, and thus one of the most important targets in the field of recycling of plastic waste. The glycolysis of PU is currently considered the most promising pathway toward industrial implementation. However, the energy consumption during the process, the cost of the excess glycol relative to PU, and the potentially reduced quality of polyol products resulting from glycol residues may still limit the speed of implementation of PU chemical recycling processes from lab to the pilot plant scale. Therefore we explore an alternative route for PU depolymerization using mechanochemistry and catalysis. In this work, we describe recovery of up to 86% of soluble polyol by mechanocatalytic methanolysis/hydrolysis of NaOH-impregnated commercial PU product (household sponge) with a Cu/MgAlOx co-catalyst below 100 ºC. The recycled polyol can serve as new raw material and has been successfully used as feedstock for the resynthesis of PU. The low reaction temperature, reduced volume of solvent, and easy separation of products could make this novel chemical recycling methodology an attractive alternative to the conventional solvolysis pathways.