Mercury (Hg) pollution poses a serious threat to the public health and ecol. environment, necessitating the urgent development of efficient and selective methods for Hg2+ removal.Herein, an ultrathin two-dimensional (2D) metal-organic framework (MOF) nanosheet decorated with extensive SO2-4 active sites was elaborately constructed.The intimate contact and robust interactions between Hg2+ and the readily accessible SO2-4 sites on the exposed surfaces of the 2D nanosheets facilitated an unparalleled adsorption capacity for Hg2+, achieving a remarkable value of 989.19 mg/g.The robust binding between Hg2+ and SO2-4 on the exposed surfaces also imparted exceptional adsorption selectivity and anti-interference capability for the 2D nanosheets, enabling practical applications in diverse real-world samples (such as acidic groundwater, mercury-oxide battery industry wastewater and petrochem. wastewater), with Hg2+ removal efficiencies surpassing 94 %.The interactions between Hg2+ and SO2-4 sites were verified by the investigations of Fourier transform IR spectroscopy, X-ray photoelectron spectrometry, zeta potential, and d. functional theory calculations, which revealed that the robust interactions between Hg2+ and SO2-4 encompass not only their direct electrostatic attractions but also intricate interactions involving Hg2+ with sulfur (mol. recognition) and oxygen atoms (chelation).These interactions cooperatively contributed to the selective and efficient capture of Hg2+ from various water samples.This study provides valuable insights into the design and construction of advanced materials for environmental remediation and metal ion capture.