The present work was aimed to evaluate the adsorption properties of activated carbons based on prickly pear seeds (PPS) and conductive polymer matrix based on polyaniline (PANI) for the removal of anionic Congo red (CR) dye from aqueous solutions. The adsorbent was prepared by polymerization of aniline in the presence of activated PPS by phosphoric acid and sodium hydroxide. The samples were characterized using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA) and the Brunauer–Emmett–Teller (BET) methods. The adsorption kinetics were studied using UV-visible (UV/Vis) spectroscopy. The characterization data suggest that the adsorption of the Congo red dye is enhanced because PANI chain molecules, which are especially accountable for removal through π—π interaction and H-bonding with the CR, are adsorbed/tethered onto the acid-activated PPS (PPSH), and thus surmount the mass transfer limitation by being best exposed to the CR-adsorbed molecule. The adsorption kinetics follows the pseudo-second order process. The correlation coefficients (R2) for Langmuir, Freundlich and Tempkin showed that the adsorption values obey Freundlich and Tempkin isotherm models. Moreover, the isotherm was most accurately described by the Freundlich model, and the maximum removal percentage was calculated to be 91.14% under optimized conditions of pH 6.6, 1 g/L of adsorbent dosage, and an initial CR dye concentration of 20 mg·L−1. Importantly, the hybrid adsorbent exhibited the highest adsorption capacity (80.15%) after five cycles of the adsorption–desorption process. Thermodynamic parameters, such as entropy changes, enthalpy changes and Gibbs free energy, were also evaluated. These results indicated that the PANI matrix can generally be better utilized for the removal of Congo red dye when appropriately dispersed on the surface of suitable support materials. These results provide a new direction to promote the separable adsorbents with increasing performance for adsorption of dye impurities from wastewater.