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Mussel inspired proteins have been demonstrated to serve as a versatile biologic adhesive with numerous applications. The present study illustrates the use of such Mussel inspired proteins (polydopamine) in the fabrication of functionalized bio‐inspired nanomaterials capable of both improving cell response and sustained delivery of model probes. X‐ray photoelectron spectroscopy analysis confirmed the ability of dopamine to polymerize on the surface of plasma‐treated, electrospun poly(ε‐caprolactone) (PCL) fiber mats to form polydopamine coating. Transmission electron microscopy images demonstrated that self‐polymerization of dopamine was induced by pH shift and that the thickness of polydopamine coating was readily modulated by adjusting the concentration of dopamine and reaction time. Polydopamine coatings were noted to affect the mechanical properties of underlying fiber mats, as mechanical …