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[Display omitted] • Novel heterojunction consisting of multishelled hollow CaTiO 3 cubes and Co 0.2 Cd 0.8 S nanoparticles was designed. • An S-scheme charge transfer route within the heterojunction was confirmed. • Mechanism for the enhanced photoactivity over Co 0.2 Cd 0.8 S/CaTiO 3 heterojunction discussed. • High H 2 -production rate achieved over heterojunction, 3.58-fold higher than Co 0.2 Cd 0.8 S. Rationally designing S-scheme heterostructures with boosted charge separation efficiency and superior redox ability is regarded as an appealing strategy to conquer the shortcomings of mono-component and conventional heterojunction photocatalysts. Herein, a novel hierarchical S-scheme heterostructured photocatalyst was constructed by integrating Co 0.2 Cd 0.8 S nanoparticles on multishelled hollow CaTiO 3 cubes to substantially improve the photocatalytic hydrogen production activity. An internal electric field (IEF) is formed at the heterojunction interfaces owing to the significant disparity in Fermi level (E F) between Co 0.2 Cd 0.8 S and CaTiO 3 , accompanied by the energy band bending, which enables the S-scheme charge transport route in the Co 0.2 Cd 0.8 S/CaTiO 3 heterostructure, as verified by electron paramagnetic resonance and theoretical calculations. Benefiting from the boosted separation efficiency and superior redox capability of photocarriers within the constructed S-scheme heterostructure, the optimized Co 0.2 Cd 0.8 S/CaTiO 3 sample exhibited a significantly improved photocatalytic hydrogen evolution rate of 8.13 mmol h−1 g−1, far exceeding that of mono-component counterparts and previously reported Co 0.2 Cd 0.8 S- or CaTiO 3 -based photocatalysts. This study is anticipated to inspire the strategic development of other economical and efficient S-scheme photocatalytic systems with enhanced H 2 evolution activity. [ABSTRACT FROM AUTHOR]