Partial detemplation of zeolites followed by desilication in alkaline medium is demonstrated as a powerful and elegant approach to design hierarchical zeolites with tailored degree of mesoporosity. This achievement, illustrated for large beta crystals, is based on the fact that the template-containing zeolite is virtually inert to Si leaching upon treatment in aqueous NaOH solutions. Partial removal of the structure-directing agent creates regions in the crystal susceptible to mesopore formation by subsequent desilication, while template-containing regions are protected from silicon extraction. Variation of the calcination temperature in the range 230–550 °C determines the amount of template removed and enables control of the extent of mesopore formation in the zeolite (20–230 m2 g−1) upon alkaline treatment. The functionality of the introduced mesoporosity in the hierarchical beta crystals is demonstrated by the improved performance in the catalytic pyrolysis of low-density polyethylene. The partial detemplation–desilication treatment enhances the tuning options of this demetallation method.