The objective of this research was to explore the changes of the pore structure and surface properties of nitric-modified lignite and base the adsorption performance on physical and chemical adsorbent characteristics. To systematically evaluate pore structure and surface chemistry effects, several lignite samples were treated with different concentrations of nitric acid in order to get different pore structure and surface chemistry adsorbent levels. A common heavy metal ion contaminant in water, Pb2+, served as an adsorbate probe to demonstrate the change of modified lignite adsorption properties. The pore structure and surface properties of lignite samples before and after modification were characterized by static nitrogen adsorption, X-ray diffraction, Scanning electron microscope, Fourier transform infrared spectroscopy, zeta potential, and X-ray photoelectron spectroscopy. The experimental results showed that nitric acid modification can increase the ability of lignite to adsorb Pb2+. The adsorption amount of Pb2+ increased from 14.45 mg·g−1 to 30.68 mg·g−1. Nitric acid reacted with inorganic mineral impurities such as iron dolomite in lignite and organic components in coal, which caused an increase in pore size and a decrease in specific surface areas. A hydrophilic adsorbent surface more effectively removed Pb2+ from aqueous solution. Nitric acid treatment increased the content of polar oxygen-containing functional groups such as hydroxyl, carbonyl, and carboxyl groups on the surface of lignite. Treatment introduced nitro groups, which enhanced the negative electrical properties, the polarity of the lignite surface, and its metal ion adsorption performance, a result that can be explained by enhanced water adsorption on hydrophilic surfaces.