Binuclear zinc complex, [Zn₂(L)(I)₂(CH₃CN)] (I) (LH₂ = 1,2-phenylenebis(azaneylylidene))bis(methaneylylidene))bis(2-methoxyphenol)) was prepared and single-crystal X-ray diffraction was used to establish the structure of complex assembly. Organic acid and base were used to functionalize the nano-porous material and then binuclear Zn complex was grafted into the modified materials. Brunauer-Emmett-Teller isotherm (BET), Nuclear Magnetic Resonance (NMR), Inductively Coupled Plasma analysis (ICP), X-ray Diffraction (XRD), Fourier transform infrared spectra (FT-IR), thermogravimetric analysis (TG), Scanning electron microscope (SEM), etc., were used to characterized the synthesized nano-catalysts to check for existence of guest moiety, structural stability of the parent and modified catalysts. Catalytic performance was noticeably enhanced post modification; without catalyst, acid/base functionalized, Zn₂ immobilized catalyst. Binuclear zinc immobilized on acid/base silica catalyst exhibited a maximum 95%, 89% conversion of piperidine, and 87% and 86% conversion of aniline respectively. Prior to the theoretical investigation the bond parameters of the binuclear zinc complex were measured experimentally. Time-dependent Density Functional Theory (TD-DFT) and Density Functional Theory (DFT) methods were used to calculate the molecule's UV–Vis absorption spectra at B3LYP as well as LANL2DZ and 6–31G(d)). LUMOs and HOMOs energy gap were determined from the electronic transitions to determine electrophilicity index (ω), softness (S), electronegativity (χ), hardness value (Ƞ), and chemical potential ($\mu )$, etc.