Lotus seed shell was employed using one-step method combining carbonization with ZnCl activation to synthesize activated carbons because of its inexpensiveness and local accessibility. The lotus seed shell-activated carbons (LSSACs) with the highest surface area (2450.8 m/g) and mesoporosity (98.6%) and the largest pore volume (1.514 cm/g) were tailored under optimum conditions as follows: impregnation ratio = 2:1, carbonization temperature = 600 °C, and time = 1.0 h. The surface Zn(II), abundant hydroxyl, and carboxyl functional groups from the activation process could result in rapid Pb(II) adsorption onto the LSSAC surface through surface complexation, ion exchange, or precipitation. The maximum monolayer adsorption capacity (q) for Pb(II) of 247.7 mg/g at 25 °C could be fitted from the Langmuir isotherm. The Gibbs free energy (△G) and positive enthalpy (△H) indicated that the adsorption process was spontaneous and endothermic, and to some extent, it was explained by the intra-particle diffusion mechanism. Our results may provide a promising way to produce activated carbons with high adsorption capacity using solid waste, which will eventually promote the environmental sustainability.