Highly ordered mesoporous molecular sieves AlMCM‐41 and a new NiO/AlMCM‐41 nanocomposite were synthesized using a sol–gel method. Fourier transform infrared (FT‐IR) spectroscopy, X‐ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), energy dispersive X‐ray spectroscopy (EDX), and N2 adsorption desorption analyses were used to examine the structure, morphology, size and phase composition of the synthesized NiO/AlMCM‐41 nanocomposites. AlMCM‐41 embedded with NiO nanoparticles was subsequently prepared using different nickel loadings in a direct synthetic route. The results show the successful deposition of NiO nanoparticles onto the framework of AlMCM‐41. AlMCM‐41 provides enormous benefits such as environmentally safe, economic viability and porosity when used as support for NiO nanoparticles. The excellent catalytic activities of AlMCM‐41 and NiO/AlMCM‐41 were investigated for the reduction of nitrophenols (4‐NP, 2‐NP) to aminophenols (4‐AP, 2‐AP) in water at ambient temperature. The best observed performance of reduction of NP with 100% conversion into analogous amino derivatives occurred within 6 min with an estimated rate constant of 0.46 min−1. The efficiency of reduction was observed to increase as a function of NiO enrichment. The NiO/AlMCM‐41 nanocomposite could be recycled and reused up to five times without noticeable change in its structure and activity. These properties make NiO/AlMCM‐41 nanocomposite an ideal platform to study various heterogeneous catalytic processes which can have application in purification, catalysis, sensing devices, and green chemistry.