In this study, a new composite, tetraethylenepentamine (TEPA), was incorporated into amino terephthalic acid-modified activated carbon (ATA@AC) through a one-pot integration of TEPA with the COOH moiety of ATA@AC. This process resulted in the creation of a TEPA@ATA@AC composite for Pb(II) removal from an aquatic environment. Several techniques, including SEM, EDX, FT-IR, TGA, XRD, and Zeta potential, were employed to emphasize the chemical composition, morphology, and thermal durability of the as-synthesized TEPA@ATA@AC composite. The impact of experimental variables on the adsorption of Pb(II) ions was studied using batch adsorption. The uptake assessment suggested that the TEPA@ATA@AC composite exhibited superior Pb(II) removal performance with high removal efficiency (97.65%) at pH = 6.5, dosage = 0.02 g, equilibrium time = 300 min, and temperature = 298 K. The isotherm data exhibited good conformity with the Langmuir isotherm model, whereas the kinetics data displayed strong agreement with both pseudo-first-order and pseudo-second-order kinetics models. This reflected that the Pb((II) uptake by the TEPA@ATA@AC composite was caused by physisorption coupled with limited chemisorption. The greatest monolayer uptake capacity of the TEPA@ATA@AC composite was 432.8 mg/g. The thermodynamic findings indicated that the Pb(II) uptake on the TEPA@ATA@AC composite was an exothermic and feasible process. After five adsorption—desorption runs, the TEPA@ATA@AC composite maintained a superior uptake capacity (83.80%). In summary, the TEPA@ATA@AC composite shows promise as a potent adsorbent for effectively removing Cr(VI) from contaminated water, with impressive removal efficiency.