Smart nano-surfaces with switchable properties are emerging as promising candidates for next-generation biomedical applications. Here we report a simple fabrication strategy for a poly(ferrocenyl methacrylate)-functionalized nano-surface that is externally redox-switchable and exhibits strong cytotoxicity toward cancer cells. Strategic positioning of poly(ferrocenyl methacrylate) on the interface of a nano-surface rather than in solution or nanoparticle cores, we envision spatially localized and tunable biological responses. The surface design is based on well-defined poly(2-(methacryloyloxy)ethylferrocenecarboxylate) (pFcMA) brushes tethered to silica nanoparticles (SiNPs) via surface-initiated reversible addition–fragmentation chain transfer (SI-RAFT) polymerization. Transmission electron microscopy (TEM) revealed polymer grafted SiNP core size varies in the range of 46–70 nm, while the grafting density of pFcMA brushes could be systematically tuned between 0.103 and 0.045 chains nm−2. Variation in monomer loading allowed systematic modulation of chain conformation from “mushroom” to “brush” regimes as confirmed by thermal and microscopic studies. The surface attached pFcMA shells displayed reversible redox behaviour, validated by cyclic voltammetry (CV), UV–visible spectroscopy, and dynamic light scattering (DLS) analysis. In human neuroblastoma and embryonic kidney cell lines, the redox-switchable poly(ferrocenyl methacrylate) coatings exhibited substantial cytotoxicity, presenting as redox-responsive nano-surface with potential applicability in stimuli-regulated guest loading and release under control. This innovative fusion of redox regulation, anticancer activity, and interfacial design reveals promising prospects in biosensing, on-demand therapeutic interfaces, and smart implant coatings.
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