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Waste plastics bring about increasingly serious environmental challenges, which can be partly addressed by their interconversion into valuable compounds. It is hypothesized that the porosity and acidity of a zeolite‐based catalyst will affect the selectivity and effectiveness, enabling a controllable and selective conversion of polyethylene (PE) into gas‐diesel or lubricating base oil. A series of embryonic, partial‐ and well‐crystalline zeolites beta with adjustable porosity and acidity are prepared from mesoporous SBA‐15. The catalysts and catalytic systems are studied with nuclear magnetic resonance (NMR), X‐ray diffraction (XRD), and adsorption kinetics and catalytic reactions. The adjustable porosity and acidity of zeolite‐beta‐based catalysts achieve a controllable selectivity toward gas‐diesel or lubricating base oil for PE cracking. With a catalyst with mesopores and appropriate acid sites, a fast escape and reduced production of cracking of intermediates are observed, leading to a significant fraction (88.7%) of lubricating base oil. With more micropores, a high acid density, and strong acid strength, PE is multiply cracked into low carbon number hydrocarbons. The strong acid center of the zeolite is confirmed to facilitate significantly the activation of hydrogen (H2), and, an in situ ammonia poisoning strategy can significantly inhibit hydrogen transfer and effectively regulate the product distribution. [ABSTRACT FROM AUTHOR]