The generation of hydrogen fuel, and wastewater treatment according to solar-driven catalysis possesses considerable prospective for establishing a carbon-neutral and ecologically sound power infrastructure. Driven by this problem, we suggest in this study, adopting a simple impregnation method, a customized association of CoAl-LDH and graphitic carbon nitride (CN), a visible light active narrow and wide band gap semiconductors. Several characterization approaches were implemented to understand the CoAl-LDH@g-C3N4 (CACN) composites' physiochemical and optical features. The CACN hetero structural forms exhibited significantly improved solar light-induced photocatalytic H2 generation and dye pollutants decomposition in contrast with pristine materials. The most effective catalyst 5 wt% CoAl-LDH@g-C3N4 (5-CACN) generated the highest hydrogen (∼430.7 μmolg−1h−1), which is 11.9-fold H2 production efficiency compared with CN and depicted significant Brilliant black dye removal efficacy via photocatalytic degradation (up to ∼79%). This was primarily ascribed to the development of the Type-II CACN heterojunctions, which promoted the separation of charges and expanded the abundance of surface-active sites while absorbing the visible spectrum of solar light.