Calcium Magnesium Aluminate (CMA) nanomaterials (NMs) were designed using a density functional theory (DFT) based materials project. Sol-gel and combustion techniques were used to prepare CMA nanoparticles and compared with characteristics and electrochemical studies with different electrodes like modified carbon paste and nickel mesh in this article. Structural characterizations using X-ray Diffraction (XRD) and Fourier Transform Infrared (FTIR) spectra were performed. Morphological characterizations using Scanning Electron Microscopy (SEM) and High-resolution Transmission Electron Microscopy (TEM) were carried out. Modified carbon paste electrodes and nickel mesh electrodes were developed using CMA NMs via sol-gel and combustion method, its electrochemical techniques such as Cyclic Voltammetry (CV), Linear Sweep Voltammetry (LSV) were compared for the sensitive detection of biomonitoring samples (i.e. uric acid, creatinine, ascorbic acid, riboflavin) and environmental contaminants (i.e. Lead nitrate and Cadmium nitrate). Specific capacitance (Csp) was calculated using CV curves for both modified carbon paste and nickel mesh electrodes found that, prepared nickel mesh electrodes by CMA NMs via sol-gel method exhibits comparatively maximum Csp value. Nickel mesh electrodes were further analysed galvanometric charge-discharge process via sol-gel and combustion technique. This report paves the way for tri-metal aluminate (CMA) design and development for electrochemical applications such as supercapacitors and sensors for the detection of various analytes.