The development of innovative materials for selective lead (Pb) capture is crucial, but regeneration research is insufficient, particularly regarding regeneration without chemical reagents. Herein, we introduce a smart, thermally regenerable MOF-based adsorbent for Pb2 + by incorporating poly(N-isopropylacrylamide) (pNIPAM) and benzo-18-crown-6 ether (B18C6) into MOF-808 (MOF-808-pNB). MOF-808-pNB could capture Pb2+ with remarkable removal efficiency (> 99.7 %), ultrafast kinetics (k2 ∼ 14.95 g mg-1 min-1), and outstanding selectivity (Kd > 1.6 × 106 mL g-1) in multi-ion mixed solutions (e.g., Li+, Ca2+, Ba2+, Cu2+, Ni2+). Importantly, this material could be easily regenerated at 45°C, showing excellent recyclability (Pb2+ adsorption and desorption ∼ 99 % after 10 cycles). Column experiments demonstrated that 1 kg material could treat 3250 L of authentic Pb-contained wastewater to meet drinking water standards (Pb < 0.01 mg/L). Mechanism studies indicate that B18C6 within the material acts as a specific site for capturing Pb2+ at 25°C, whereas pNIPAM shrinks thermoresponsively to a hydrophobic state at 45°C. These alterations introduce steric hindrance and repulsion, combined with exothermic properties of B18C6, collectively enabling efficient Pb2+ desorption. This work highlights the potential of thermoresponsive MOF-808-pNB for Pb2+ removal and provides a reference for the design of stimuli-responsive materials aimed at water purification.