Water contamination becomes one of the most high-priority environmental concerns, calling for the efficient treatment techniques. Bionanocomposites can be robust adsorbents, but the synthesis requires toxic chemicals or energy consuming and cause the secondary pollution. Green nanocomposites can be biogenically synthesized using the plant extract to end up with a critically safe strategy. Herein, we used the flower extract of Combretum indicum plant as a bio-based reductant and carbonaceous source for the green CuO@C nanocomposite. This green nanoadsorbent obtained a specific surface area of 17.33 m2/g, good crystallinity, and functional group-containing surface, i.e., -OH and -CONH-. We also conducted the optimization of parameters, i.e., concentration, CuO@C dose, pH, time, and temperature, and reached removal efficiencies towards malachite green (MG, 83.23%), Congo red (CR, 84.60%), brilliant blue (BB, 71.39%), and methylene blue (MB, 23.67%). The maximum adsorption capacities were found as ordered, MG (46.387 mg/g) > MB (23.154 mg/g) > BB (22.8 mg/g) > CR dye (11.063 mg/g). Through the intra-particle diffusion kinetic model, MG and BB adsorption endured a three-step process, while CR and MB adsorption was a two-step process. The recyclability of the green CuO@C nanocomposite was three cycles with 67.54% for the final cycle of BB removal. Moreover, the nanoadsorbent displayed a high stability, checked by X-ray diffraction, FT-IR analysis, EDX spectra, and SEM images. It is recommended that the green CuO@C nanocomposite biosynthesized using the Combretum indicum flower extract can be a good alternative for the dye treatment from wastewater.