This study presents the fabrication of a novel porous composite of graphene oxide-montmorillonite (GO-MMT) through the modification of montmorillonite using the freeze-drying method for the purpose of Pb removal. The characterization of the GO-MMT composite was conducted using scanning electron microscopy, Fourier transform infrared spectrometry, and X-ray diffraction. The results from batch adsorption experiments revealed that the GO-MMT composite exhibited a superior capacity for Pb removal compared to MMT. Furthermore, a single factor experiment confirmed that the dosage of the GO-MMT composite or GO, pH, temperature, and reaction time all significantly influenced the adsorption of Pb by the GO-MMT composite, MMT, or GO. This superiority can be attributed to the presence of oxygen-containing functional groups, the site-blocking effect, and the ion exchange mechanism exhibited by the GO-MMT composite.