<p>The efficient chemical recycling of polyethylene terephthalate (PET) remains a key challenge for sustainable polymer management. Herein, we report a series of tunable titanate nanostructured catalysts prepared via NaOH-controlled hydrothermal synthesis of TiO₂, which enables systematic tuning of catalyst morphology and surface area. Among them, the optimized TN-10 catalyst exhibits an interconnected nanotubular architecture with a high specific surface area (~ 184 m² g^-1). TN-10 efficiently catalyzes PET methanolysis under moderate reaction conditions, delivering 84% PET conversion with a dimethyl terephthalate (DMT) yield of 94%, and performs well for both virgin and post-consumer PET. The catalyst is also effective for the depolymerization of polybutylene terephthalate (PBT), affording DMT in 91% yield. Furthermore, TN-10 shows good compatibility with a range of alcohols in the presence of K₂CO₃, enabling selective alcoholysis to the corresponding diesters. TN-10 retains activity over five cycles and performs reliably in gram-scale reactions. This study provides insights into structure-activity relationships in titanate catalysts for efficient polyester depolymerization.</p> Graphical Abstract <p></p>