This study introduces a new and bio-friendly adsorbent based on natural and cetyltrimethylammonium chloride (CTAC)-modified adsorbent prepared from wheat straw residues for the removal of Congo red (CR) and tartrazine azo-anionic dyes from aqueous solution. The adsorbent was characterized by thermogravimetric analysis (TGA), calorimetric differential (DSC), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM/EDX), and pH point of zero charge (pHPZC) techniques. It was found that decreasing the adsorbent dose and increasing the initial concentration favors the removal of tartrazine and Congo red. Tartrazine adsorption capacities were 2.31 mg/g for the cellulose extracted from wheat residues (WC) and 18.85 mg/g for the modified wheat residue cellulose (MWC) for tartrazine as well as 18.5 mg/g for WC and 19.92 for MWC during Congo red (CR) adsorption, respectively. Increasing the initial and decreasing the adsorbent dose concentration favored the adsorption process. From time effect analysis, it was found that the equilibrium time was reached at 120 min when modified wheat cellulose was used and at 480 min when wheat cellulose was used. The kinetics of adsorption were described by pseudo-second-order in all cases with R2 > 0.95. The obtained data equilibrium from this research was well-fitted by the Freundlich isotherm model.