Starburst-like nanogels from vinyl-functionalized poly(lactic acid) and silk sericin via Aloe vera gel extract–mediated self-assembly: Toward multifunctional natural polymer nanomaterials

Abstract

Nanogels based on crosslinked polymer networks have emerged as promising candidates for drug delivery owing to their tunable nanostructure, high water content, and inherent biocompatibility. In this study, sustainable nanogels were synthesized via redox-initiated polymerization from vinyl-functionalized poly(lactic acid) macromers (PLAM) and silk sericin crosslinkers (SSC), incorporating Aloe vera gel extract (AV) as a multifunctional, carbohydrate- and protein-rich additive. Multimodal characterization—including elemental mapping, X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD)—revealed a dynamic self-assembly into starburst-like nanostructures under aqueous conditions. This morphology, prominently observed by day 3, arises from nanoscale phase separation between hydrophobic PLAM and hydrophilic SSC, while AV-derived polysaccharides and glycoproteins facilitate extensive hydrogen bonding and hydration-induced matrix rearrangement. The resulting architecture consists of a compact hydrophobic core with radiating arms embedded in hydrated amorphous domains. Protein release profiles exhibited an initial burst phase followed by sustained release, confirming efficient encapsulation and diffusion-controlled delivery. These findings highlight the role of supramolecular interactions and hydrophilic–hydrophobic balance in directing nanoscale morphology and drug release kinetics, positioning these starburst-like nanogels as sustainable platforms for controlled drug delivery and regenerative medicine applications.