Abstract Nicotinamide adenine dinucleotide NAD(P)H is a prolific cofactor in oxidoreductases biochemistry, but its high cost and the stoichiometric amounts motivates significant research for establishing efficient solutions for regenerating NAD(P)H from NAD(P) + . This study presents nanoparticles of gold/layered double hydroxides (AuNPs/LDH) as nanoplatforms with highly efficient photocatalytic response for solar‐light promoted NADH regeneration. The novel photocatalysts are obtained via self‐assembling of ZnAlLDH and AuNPs by using the manifestation of the “structural memory” of the anionic clay in gold salt solution. The chemical composition, structural, optical and nanotextural features of AuNPs/LDH have been assessed by transmission electron microscopy (TEM), energy dispersive X‐Ray Spectroscopy (EDX), powder X‐ray diffraction (XRD), and UV‐Vis Spectroscopy (UV‐Vis). It was found that, at pH 8 and in the presence of flavin mononucleotide (FMN) as a mediator and using water as an electron donor, the regeneration the NADH under solar light is defined by a rate of 20.5 μM/h. Furthermore, the regenerated NADH cofactor is tested in presence of Horseradish Peroxidase (HRP) enzyme to promote the hydrogen peroxide reduction.