A series of hybridized charged membrane materials containing carboxyl and silyl groups were prepared via the epoxy ring-opening reaction and sol–gel methods using 3-glycidoxypropyltrimethoxysilane (WD-60) and polyethylene glycol 6000 (PEG-6000) as raw materials and DMF as a solvent. Scanning electron microscopy (SEM), fourier transform infrared spectroscopy (FTIR), and thermal gravimetric analyzer/differential scanning calorimetry (TGA/DSC) analysis showed that the heat resistance of the polymerized materials could reach over 300 °C after hybridization. A comparison of the results of heavy metal lead and copper ions’ adsorption tests on the materials at different times, temperatures, pHs, and concentrations showed that the hybridized membrane materials have good adsorption effects on heavy metals and better adsorption effects on lead ions. The maximum capacity obtained from optimized conditions for Cu2+and Pb2+ions were 0.331 and 5.012 mmol/g. The experiments proved that this material is indeed a new environmentally friendly, energy-saving, high-efficiency material. Moreover, their adsorptions for Cu2+and Pb2+ions will be evaluated as a model for the separation and recovery of heavy metal ions from wastewater.