This study reports a novel intrabridging strategy to improve the antifouling performance of a thin-film composite (TFC) membrane. We demonstrate that the addition of Ca2+ during the interfacial polymerization reaction led to the formation of stable Ca2+-carboxyl complexes within the polyamide rejection layer. This intrabridging of carboxyl groups by Ca2+ effectively sequestrated them, reducing their availability for binding divalent metal ions in the aqueous solution and for forming foulant-metal-membrane interbridges. Membrane fouling and cleaning experiments confirmed improved flux stability and fouling reversibility for the Ca2+ modified membranes. The greatly enhanced antifouling performance of these membranes, together with their better surface hydrophilicity and greater water permeability, makes the intrabridging approach highly attractive in overcoming the classical permeability-selectivity-antifouling trade-off. Our findings pave a new direction for synthesizing high-performance TFC membranes.