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The effects of heterogeneous reactions between river‐borne particles and the carbonate system were studied in the plumes of the Mississippi and Brazos rivers. Measurements within these plumes revealed significant removal of dissolved inorganic carbon (DIC) and total alkalinity (TA). After accounting for all known DIC and TA sinks and sources, heterogeneous reactions (i.e., heterogeneous CaCO₃precipitation and cation exchange between adsorbed and dissolved ions) were found to be responsible for a significant fraction of DIC and TA removal, exceeding 10% and 90%, respectively, in the Mississippi and Brazos plume waters. This finding was corroborated by laboratory experiments, in which the seeding of seawater with the riverine particles induced the removal of the DIC and TA. The combined results demonstrate that heterogeneous reactions may represent an important controlling mechanism of the seawater carbonate system in particle‐rich coastal areas and may significantly impact the coastal carbon cycle.