Multifunctional nanofibrous architectures have attracted
extensive
attention for biomedical applications due to their adjustable and
versatile properties. Electrospun fabrics stand out as key building
blocks for these structures, yet improving their mechanobiological
and physicochemical performance is a challenge. Here, we introduce
biodegradable engineered hydrophobic/hydrophilic scaffolds consisting
of electrospun polylactide nanofibers coated with drug-eluting synthetic
(poly(vinyl alcohol)) and natural (starch) polymers. The microstructure
of these composite scaffolds was tailored for an increased hydrophilicity,
optimized permeability, water retention capacity of up to 5.1 g/g,
and enhanced mechanical properties under both dry and wet conditions.
Regarding the latter, normalized tensile strengths of up to 32.4 MPa
were achieved thanks to the improved fiber interactions and fiber-coating
stress transfer. Curcumin was employed as a model drug, and its sustained
release in a pure aqueous medium was investigated for 35 days. An
in-depth study of the release kinetics revealed the outstanding water
solubility and bioavailability of curcumin, owing to its complexation
with the hydrophilic polymers and further delineated the role of the
hydrophobic nanofibrous network in regulating its release rate. The
modified curcumin endowed the composites with antioxidant activities
up to 5.7 times higher than that of free curcumin as well as promising
anti-inflammatory and bacteriostatic activities. The cytocompatibility
and cell proliferation capability on human dermal fibroblasts also
evidenced the safe use of the constructs. Finally, the fabrics present
pH-responsive color-changing behavior easily distinguishable within
the pH range of 5–9. Thus, these designs offer a facile and
cost-effective roadmap for the fabrication of smart multifunctional
biomaterials, especially for chronic wound healing.