Traditional aerogels lack specific functional groups for the adsorption of Pb2+, which results in a low adsorption capacity and limits the application scope. Novel porous pectin-based aerogels (PPEAs) were prepared by incorporating polyethylenimine (PEI) using ethylene glycol diglycidyl ether (EGDE) as a cross-linker for the removal of Pb2+ from water. The cross-linking mechanism, morphology, mechanical strength, thermal stability, adsorption properties, and mechanism of the aerogels were investigated. The aerogels possessed several desirable features, such as a large maximum Pb2+ adsorption capacity (373.7 mg/g, tested at pH 5.0), ultralight (as low as 63.4 mg/cm3), high mechanical strength (stress above 0.24 MPa at 50% strain), and easy recyclability. Meanwhile, the equilibrium adsorption data was well described by the Langmuir–Freundlich (Sips) model and the kinetic adsorption process was well fitted using the pseudo-second-order model. The donor groups, such as -NH2, and oxygen-containing functional groups were responsible for the Pb2+ adsorption, which was confirmed by the FTIR and XPS analysis. The excellent characteristics mean that PPEAs are highly effective adsorbents in the remediation of lead-containing wastewater.