Electrochemical upcycling of polyethylene terephthalate (PET) hydrolysate into value‐added chemicals presents a sustainable solution to address plastic pollution and energy demands. However, conventional noble metal‐based electrocatalysts often suffer from rapid deactivation due to surface oxidation and intermediate poisoning, while conventional pulse strategies exhibit compromised efficiency during resting potentials. Herein, an alternating (ALT) pulse strategy is developed utilizing a mesoporous high‐entropy film (m‐HEA/NF) bifunctional catalyst that enables continuous anodic production of glycolic acid (GA) coupled with cathodic H ₂ evolution. The system achieves 97% Faradaic efficiency for GA (FE _GA ) and ≈100% FE _H2 at 250 mA cm ⁻² with GA and H ₂ production rates (PR _GA and PR _H2 ) of 2.284 mmol cm ⁻² h ⁻¹ and 108 mL cm ⁻² h ⁻¹ , respectively, representing a significant improvement over the conventional pulse strategy. Notably, the membrane‐free flow system delivers a current of 2 A with a PR _GA of 15.114 mmol cm ⁻² h ⁻¹ , demonstrating remarkable potential for industrial implementation. In situ spectroscopic analysis reveals that the ALT pulse strategy effectively mitigates metal oxidation and prevents intermediate accumulation through periodic regeneration of active sites, while the alternating anodic/cathodic cycles eliminate resting periods to enhance operational efficiency. The work establishes a universal paradigm for sustainable electrosynthesis, integrating plastic valorization with energy‐efficient H ₂ production.

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