For many years, research scientists have aided communities in their tremendous eﬀorts towards environmental remediation. Due to their high physical and chemical stability, metal oxide nanoparticles (NPs) have been used as metal catalysts to remedy this issue. This article reviews green approaches for the synthesis of metal oxide nanoparticles, in aqueous bio-reductive polyphenols from punica granatum peel extract and the degradation of organic pollutants. The bimetallic nanocomposite of face-centred cubic NiO/MgO pseudocapacitors were successfully prepared via the polyphenols of punica granatum peel extracts. X-ray diﬀraction spectroscopy (XRD) successfully provide evidence of polycrystalline face-centre cubic nanocomposite (high crystallinity index (Icry) > 1) while revealing their interplanar distance. The spherical and irregular particle distribution of the binary NiO/MgO nanocomposite (at diﬀerent calcination temperatures) was assessed by high resolution-TEM. FTIR, GC–MS and EDS provided evidence of the proposed mechanism during coordination between polyphenols and metal precursors. The popular “egg box model” is referred to in the case of polyphenols-metal interaction. The unique feature of two consecutive chelation site per repeat that provides a favourable entropic contribution to the inter-chain association is produced by this model governed by electrostatic interactions. Based on the obtained results, new structural models of Ni2+/Mg2+-polyphenols (punicalagin) complexes were proposed. UV–vis and Cyclic voltammetry conﬁrmed the growth and band gap energies of the nanocomposite. NiO/MgO nanocomposite was found to be excellent photocatalysts for the degradation of methylene orange and methylene blue under the illumination of artiﬁcial light irradiation. The experiments demonstrated that MB in aqueous solution was more eﬃciently photo-degraded (87%) than MO (73%) using NiO/MgO nanocomposite as photocatalysts within 10 min of exposure. Conclusively, the nanocomposite was found to be more eﬃcient compared to other reported oxides.