The leather tanning industry is releasing Chrome Hexavalent Cr(VI), resulting in detrimental consequences and requiring remedial intervention. This study investigated the possible application of watermelon peels as a bio-adsorbent for removing Cr(VI) from water-based solutions, using watermelon peels in their normal state and watermelon peel nanoparticles. Transmission electron microscopy (TEM) and FT-IR spectroscopy were used to characterize watermelon peels. The tannery wastewater and standard Cr(VI) water solutions were used in adsorption tests with a range of adsorbent amounts, contact times, pH 4, and temperatures (25 °C). The residual Cr(VI) was determined using inductively coupled plasma (ICP). The Langmuir isotherm's model fits the adsorption data perfectly. Results showed that the watermelon peels of normal powder and nanopowder were removed up to 77.61% and 100%, respectively, at an aqueous solution of 400 ppm of Cr(VI), pH 4, the amount of adsorbent was 8 gram/liter, the temperature was 25 °C, and the contact time was 120 minutes. Additionally, the watermelon peels of normal powder and nanopowder were removed up to 62.31 and 74.45%, respectively, at an aqueous solution of 600 ppm of Cr(VI), pH 4, the amount of adsorbent was 8 gram/liter, the temperature was 25 °C, and the contact time was 120 minutes. Therefore, we recommend using nano watermelon peels since they improve adsorbing Cr(VI) efficiency in a shorter period compared to regular-sized peels. Furthermore, the isotherm model from Langmuir and the data on adsorption are strongly associated.