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Removing organic dyes from contaminated wastewater resulting from industrial effluents with a cost-effective approach addresses a major global challenge. The adsorption technique onto carbon-based materials and metal oxide is one of the most effective dye removal procedures. The current work aimed to evaluate the application of calcium oxide-doped carbon nitride nanostructures (CaO-g-C₃N₄) to eliminate basic fuchsine dyes (BF) from wastewater. CaO-g-C₃N₄ nanosorbent were obtained via ultrasonication and characterized by scanning electron microscopy, X-ray diffraction, TEM, and BET. The TEM analysis reveals 2D nanosheet-like nanoparticle architectures with a high specific surface area (37.31 m²/g) for the as-fabricated CaO-g-C₃N₄ nanosorbent. The adsorption results demonstrated that the variation of the dye concentration impacted the elimination of BF by CaO-C₃N₄ while no effect of pH on the removal of BF was observed. Freundlich isotherm and Pseudo-First-order adsorption kinetics models best fitted BF adsorption onto CaO-g-C₃N₄. The highest adsorption capacity of CaO-g-C₃N₄ for BF was determined to be 813 mg. g⁻¹. The adsorption mechanism of BF is related to the π-π stacking bridging and hydrogen bond, as demonstrated by the FTIR study. CaO-g-C₃N₄ nanostructures may be easily recovered from solution and were effectively employed for BF elimination in at least four continuous cycles. The fabricated CaO-g-C₃N₄ adsorbent display excellent BF adsorption capacity and can be used as a potential sorbent in wastewater purification.