{Reference Type}: Journal Article {Title}: The surface charge of electroactive materials governs cell behaviour through its effect on protein deposition. {Author}: Rodriguez-Lejarraga P;Martin-Iglesias S;Moneo-Corcuera A;Colom A;Redondo-Morata L;Giannotti MI;Petrenko V;MonleĆ³n-Guinot I;Mata M;Silvan U;Lanceros-Mendez S; {Journal}: Acta Biomater {Volume}: 184 {Issue}: 0 {Year}: 2024 Aug 29 {Factor}: 10.633 {DOI}: 10.1016/j.actbio.2024.06.039 {Abstract}: The precise mechanisms underlying the cellular response to static electric cues remain unclear, limiting the design and development of biomaterials that utilize this parameter to enhance specific biological behaviours. To gather information on this matter we have explored the interaction of collagen type-I, the most abundant mammalian extracellular protein, with poly(vinylidene fluoride) (PVDF), an electroactive polymer with great potential for tissue engineering applications. Our results reveal significant differences in collagen affinity, conformation, and interaction strength depending on the electric charge of the PVDF surface, which subsequently affects the behaviour of mesenchymal stem cells seeded on them. These findings highlight the importance of surface charge in the establishment of the material-protein interface and ultimately in the biological response to the material. STATEMENT OF SIGNIFICANCE: The development of new tissue engineering strategies relies heavily on the understanding of how biomaterials interact with biological tissues. Although several factors drive this process and their driving principles have been identified, the relevance and mechanism by which the surface potential influences cell behaviour is still unknown. In our study, we investigate the interaction between collagen, the most abundant component of the extracellular matrix, and poly(vinylidene fluoride) with varying surface charges. Our findings reveal substantial variations in the binding forces, structure and adhesion of collagen on the different surfaces, which collectively explain the differential cellular responses. By exposing these differences, our research fills a critical knowledge gap and paves the way for innovations in material design for advanced tissue regeneration strategies.