AbstractCatalytic hydrogenolysis is a promising approach to transform waste plastic into valuable chemicals. However, the transformation of N-containing polymers, such as polyamides (i.e. nylon), remains under-investigated, particularly by heterogeneous catalysis. Here, we demonstrate the hydrogenolysis of various polyamides catalysed by platinum-group metal nanoparticles supported on CeO2. Ru/CeO2 and Pt/CeO2 are both highly active but display different selectivity; Ru/CeO2 is selective for the conversion of all polyamides into water, ammonia, and methane, whereas Pt/CeO2 yields hydrocarbons retaining the carbon backbone of the parent polyamide. Density functional theory computations illustrate that Pt nanoparticles require higher activation energy for carbon−carbon bond cleavage than Ru nanoparticles, rationalising the observed selectivity. The high activity and product selectivity of both catalysts was maintained when converting real-world polyamide products, such as fishing net. This study provides a mechanistic basis for heterogeneously catalysed polyamide hydrogenolysis, and a new approach to the valorisation of polyamide containing waste.