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Developing effective catalysis to address end-of-life Nylon pollution is urgent yet remains underdeveloped. Nylon-6 is a resilient synthetic plastic and a major contributor to ocean pollution. Here, we report a metallocene catalytic system based on earth-abundant early transition and lanthanide metals that mediates Nylon-6 depolymerization at unprecedented rates up to 810 (ε-caprolactam)$ mol(Cat.)1$h1 at 240C in R99% yield. This solventless process operates with catalyst loadings as low as 0.04 mol % at temperatures as low as 220C—themildest Nylon-6 depolymerization conditions reported to date. This metallocene catalysis can be carried out in a simulated continuous process, and the resulting ε-caprolactam can be re-polymerized to higher-quality Nylon-6. Experimental and DFT analyses identify effective depolymerization pathways involving catalytic intra-Nylon-chain ‘‘unzipping’’ assisted by p-ligand effects and inter-chain ‘‘hopping.’’ A robust chelating ansa-yttrocene is particularly effective in depolymerizing diverse commodity end-of-life articles, such as fishing nets, carpets, clothing, and plastic mixtures.