Loess is a typical natural mineral particle distributed widely around the world, and it is inexpensive, readily accessible, and harmless to the environment. In this study, loess was modified by surface grafting copolymerization of functional monomers, such as acrylic acid, N-vinyl pyrrolidone, and N,N-methylenebisacrylamide as a cross-linking agent, which afforded a novel loess-based grafting copolymer (LC-PAVP). After being characterized by scanning electron microscopy, thermal gravimetric analysis and Fourier-transform infrared spectroscopy, its adsorption capacity and mechanism of removing lead ions (Pb2+) were investigated. With the study of the optimal experimental conditions, it was demonstrated that the removal rate of Pb2+ by LC-PAVP can reach up to 99.49% in 60 min at room temperature. It was also found that the kinetic characteristics of the adsorption capacity due to the pseudo-second-order kinetic model and the thermodynamics conformed well with the Freundlich model. In summary, as a lost-cost and eco-friendly loess-based adsorbent, LC-PAVP is a good potential material for wastewater treatment.