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The design of novel materials for sulfur dioxide (SO2) capture and conversion with considerable efficiency under mild conditions is of great significance for human health and environmental protection yet highly challenging. Herein, we report a series of triazine‐based multicomponent metallacages via coordination‐driven self‐assembly of 2,4,6‐tri(4‐pyridyl)‐1,3,5‐triazine, cis‐Pt(PEt3)2(OTf)2 and different tetracarboxylic ligands. As the increase of the length of the tetracarboxylates, the structures of the metallacages change from pyramids to extended octahedrons. Owing to their N‐rich structure, these metallacages are further used for selective SO2 capture, showing good adsorption capacity and remarkable SO2/CO2 selectivity in ambient conditions, suggesting their potential applications toward real flue gas desulfurization. The metallacages are further employed for the conversion of SO2 into value‐added compounds, showing exceptional efficiency even dilute SO2 is used as the reactant. This study represents a type of structure‐tunable triazine‐based metallacages for SO2 capture and conversion, which will pave the way on the applications of metal‐organic complexes for gas adsorption. [ABSTRACT FROM AUTHOR]