This article describes an easy and simple method to remove a toxic Acid Red dye from aqueous solution. Ternary poly(O-toluidine)/graphene oxide/chitosan P(OT)/GO/CS nanocomposites (NCs) were fabricated by an oxidative polymerization technique to remove Acid Red (A.R.) dye from aqueous solutions using solid-phase extraction. The P(OT)/GO/CS NCs exhibit a metal sieve-like structure consisting of GO nanosheets and a core shell-shell porous structure, which provides several adsorption sites and channels for the transport of dye molecules. FTIR, XRD, RAMAN, TEM, SEM, BET, and TGA-DTG investigations were carried out on NCs. To investigate the removal effectiveness of the NCs using adsorbent dose, pH and solution temperature, shaking time, and ionic strength. Experimental adsorption findings, utilizing 15 mg of solid-phase NCs, can remove the majority of the A.R. dye in 75 min at pH 2.0 with an adsorption efficiency and an adsorption capacity of 99.6% and 169.5 mg/g, respectively. The pseudo-second-order kinetic model best captures the adsorption process of A.R. dye on the NC solid phase, according to experimental data. Thermodynamically, the removal process was endothermic, spontaneous, and associated with increasing randomness. Finally, NCs were tested by removing A.R. dye from real samples. NCs removed A.R. dye from aqueous solutions for four cycles.