<p>Development of polymers with underwater self-healing and antifouling properties is crucial, particularly in harsh marine environments. In this study, polydimethylsiloxane (PDMS)-based antifouling polymers with tunable self-healing capabilities in aqueous conditions were fabricated by incorporating amphiphilic segments and Fe³⁺-catechol dynamic coordination crosslinking. The microphase formed within the PDMS matrix imparted static antifouling properties to the coatings. The mechanical properties of the damaged sample were restored at room temperature in an aqueous environment for 24 h, achieving a self-healing efficiency of almost 100%. The synthesized material exploited the dynamic coordination between Fe³⁺ and catechol to facilitate underwater self-healing. No bacterial adhesion was observed at the scratch site after the coating was repaired. This material enables the long-term antifouling and autonomous repair of marine vessels and sensors, thereby reducing maintenance costs.</p>