In this study, a low-cost bioadsorbent aluminum metal blended with groundnut shell activated carbon material (Al-GNSC) was used for Cr(VI) adsorption from aqueous solutions. Al-GNSC was prepared and characterized using Fourier transform infrared spectrometer (FT-IR), scanning electron microscopic (SEM) and X-ray diffraction (XRD) to determine its surface morphology. Batch studies were performed and the optimum conditions for maximum Cr(VI) removal (of 94.2%) were found at pH 4.0, initial concentration 100 mg/L, adsorbent dosage 8 g/L of Cr(VI) solution, and time of contact 50 min. Moreover, the Langmuir isotherm model (maximum adsorption capacity of 13.458 mg/g) was the best fit and favored the mono-layered Cr(VI) adsorption. The kinetic studies reveal that the pseudo-second-order model was the best fit and favored chemisorption as the rate-limiting step. The desorption study revealed that Cr(VI) leached with sodium hydroxide solution acted as a regenerating agent. It is proved that Al-GNSC removes the Cr(VI) content in groundwater samples. The methodology developed using the Al-GNSC adsorbent as an alternative for the adsorption of Cr(VI) ions is remarkably successful in this study.