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Building long-lasting antimicrobial and clean surfaces is one of the most effective strategies to inhibit bacterial infection, but obtaining an ideal smart surface with highly efficient, controllable, and regenerative properties still encounters many challenges. Herein, we fabricate an ultrathin brush–hydrogel hybrid coating (PSBMA-P(HEAA-co-METAC)) by integrating antifouling polyzwitterionic (PSBMA) brushes and antimicrobial polycationic (P(HEAA-co-METAC)) hydrogels. The smart bacterial killing–releasing properties can be achieved independently by the opposite volume and conformation changes between the swelling (shrinking) of P(HEAA-co-METAC) hydrogel layer and the shrinking (swelling) of PSBMA brushes. The friction test reveals that both METAC and SBMA components support great lubrication. By tuning the initial organosilane (BrTMOS:KH570) ratios, the prepared PSBMA-P(HEAA-co-METAC) coating exhibits different antibacterial abilities from single “capturing–killing” to versatile “capturing–killing–releasing.” Most importantly, 99% of the bacterial-releasing rate can be easily achieved via 0.5 M NaCl treatment. This smart surface not only possesses long-lasting antibacterial performance, only ∼1.09 × 105 cell·cm−2 bacterial residue even after 72 h exposure to bacteria solutions, but also can be regenerated and triggered between water and salt solution multiple times. This work provides a new way to fabricate antibacterial smart hydrogel coatings with bacterial “killing–releasing” functions and shows great potential for biomedical applications.