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A well-designed two-dimensional 2D/2D architecture was constructed by coupling oxygen-vacancy-rich trimetallic CoAlLa layered double hydroxide (CoAlLa-LDH) with titania-sandwiched Ti₃C₂ MXene multilayers to achieve enhanced photocatalytic CO₂ reduction. First, through a controlled etching process, in situ anatase/rutile-phase titania was grown over Ti₃C₂ multilayers with a controlled morphology. In the next stage, through controlled growth, a highly active oxygen-vacancy-rich ternary CoAlLa-LDH was formed in the presence of La³⁺ to create coordinatively unsaturated metal centers for enhancement of reductive sites. An intimate contact between the trimetallic CoAlLa layered double hydroxide (CoAlLa-LDH) and Ti₃C₂T_x with a unique 2D/2D hierarchical architecture was achieved. This step (S)-scheme heterojunction provided pathways to effectively stimulate the photoinduced electron–hole separation …