New self-healing agents that can chemically bind seawater ions invading cracked cementitious materials were proposed. The potential of self-healing and binding of seawater ions were investigated by thermodynamic modeling. It was found that CaO-NaAlO₂ and CaO-metakaolin agents can have Cl⁻, SO₄²⁻ and Mg²⁺ chemically bound by reacting with sea water to form Friedel's salt, Kuzel's salt, ettringite and hydrotalcite. The removal of Cl⁻ from seawater firstly increased and then decreased with the increase of Ca/Al molar ratio in both agents, while the removal of Mg²⁺ and SO₄²⁻ were hardly influenced and approximated 100%. Because NaAlO₂ dissolves and releases Al(OH)₄⁻ rapidly, precipitates binding Cl⁻, SO₄²⁻ and Mg²⁺ were formed fast. In comparison, the reaction of metakaolin binding aggressive ions occurred after 3 days. Because of the faster reaction and the capacity to make [Cl⁻]/[OH⁻] lower in the solution, CaO-NaAlO₂ would be more efficient for self-healing and mitigating reinforcement corrossion than CaO-metakaolin.