Selective elimination of sulfur dioxide is significant in flue gas desulfurization and natural gas purification, yet developing adsorbents with high capture capacity especially at low partial pressure as well as excellent cycling stability remains a challenge. Herein, a family of isostructural gallate-based MOFs with abundant hydrogen bond donors decorating the pore channel was reported for selective recognition and dense packing of sulfur dioxide via multiple hydrogen bonding interactions. Multiple O···H-O hydrogen bonds and O···H-C hydrogen bonds guarantee SO2 molecules are firmly grasped within the framework, and appropriate pore apertures afford dense packing of SO2 with high uptake and density up to 1.86 g cm-3, which is evidenced by dispersion-corrected density functional theory calculations and X-ray diffraction resolution of a SO2-loaded single crystal. Ultrahigh adsorption uptake of SO2 at extremely low pressure (0.002 bar) was achieved on Co-gallate (6.13 mmol cm-3), outperforming all reported state-of-the-art MOFs. Record-high IAST selectivity of SO2/CO2 (325 for Mg-gallate) and ultrahigh selectivity of SO2/N2 (>1.0 × 104) and SO2/CH4 (>1.0 × 104) were also realized. Breakthrough experiments further demonstrate the excellent removal performance of trace amounts of SO2 in a deep desulfurization process. More importantly, M-gallate shows almost unchanged breakthrough performance after five cycles, indicating the robust cycling stability of these MOFs.