Dual-function antibacterial surfaces have exhibited promising potential in addressing implant-associated infections. However, both bactericidal and antifouling properties need to be further improved prior to practical uses. Herein, we report the preparation and properties of a linear block copolymer coating (LP-KF) and a single-chain nanoparticle coating (NP-KF) with poly(ethylene glycol) (PEG) and cationic polypeptide segments. NP-KF with cyclic PEG segments and densely charged polypeptide segments was expected to display improved bactericidal and antifouling properties. LP-KF was prepared by the combination of ring-opening polymerization of N-carboxyanhydride (NCA) monomers and subsequent deprotection. NP-KF was prepared by intramolecular cross-linking of LP-KF in diluted solutions. Both LP-KF- and NP-KF-coated PDMS surfaces were prepared by dipping with polydopamine-coated surfaces. They showed superior in vitro bactericidal activity against both Staphylococcus aureus and Escherichia coli with >99.9% killing efficacy, excellent protein adsorption resistance, antibacterial adhesion, and low cytotoxicity. The NP-KF coating showed higher bactericidal activity and antifouling properties than its linear counterpart. It also showed significant anti-infective property and histocompatibility in vivo, which makes it a good candidate for implants and biomedical device applications.