Nitroterephthalic acid (NTA)-based supramolecular Co(II)/Cu(II) metallogels were precisely achieved. NTA as the low molecular weight gelator is stoichiometrically combined with respective metal salts to construct Co-NTA and Cu-NTA metallogels in N,N′-dimethylformamide (DMF) medium. The mechanoelastic properties of both metallogels have been meticulously established through the assessment of rheological parameters. The microstructural arrangements within the xerogel samples are intricately elucidated through field emission electron scanning microscopy (FESEM), and this depicts distinct interconnected stacked-like morphological configurations within the supramolecular metallogels. Verification of persisting elements contributing to the metallogel formation is achieved through comprehensive EDX elemental analyses. FTIR spectroscopic analyses dictate the signature of noncovalent interactions for offering an individual stable metallogel network. The possible major repeating unit within the metallogel network is ascertained with the utmost precision through exhaustive ESI mass spectral analyses. The semiconducting behavior of the fabricated metallogels has also been executed. Remarkably, these metallogels exhibit nonlinear J−V characteristics, accompanied by rectification ratios of 102.82 (Co-NTA) and 211.52 (Cu-NTA), underscoring exceptional charge transport attributes for both metallogels. Notably, insights into the Schottky diode parameters of both metallogels and Cu-NTA material display enhanced effective interface mobility, conductivity, and transit time, collectively implying an improved conduction mechanism.