This paper proposes a sonochemical approach to the nanostructuring of Al/Ni catalyst with high content of accessible Ni centers and a high reusability. The surface and bulk composition as well as pore size distribution of this catalyst are controlled synergistically by adjusting the ultrasound intensity in aqueous solution. Sonochemical activation of Al/Ni alloy leads to formation of mesoporous Al/Ni metallic based frameworks with surface area up to 125 m2 g−1, and regular distribution of nickel active center in the porous matrix. One of the opportunities of porous Al/Ni catalyst is that due to a time-resolved controllable formation of protective oxide layer it can be stored and handled under air in comparison to traditional Raney catalysts which need inert conditions. The Al/Ni catalyst is characterized by scanning electron microscopy (SEM), electron diffraction spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), confocal scanning fluorescence microscopy (CSFM), solid-state NMR experiments, and powder X-ray diffraction analysis (PXRD). The catalytic activity was investigated for the hydrogenation of acetophenone.