Hierarchical Inorganic–Organic Nanocomposites Possessing Amphiphilic and Morphological Complexities: Influence of Nanofiller Dispersion on Mechanical Performance

Novel nanocomposites possessing ternary compositions and complex morphologies have been prepared from amphiphilic crosslinked hyperbranched fluoropolymer–poly(ethylene glycol) (HBFP–PEG) in the presence of pristine and chemically functionalized nanoscopic fillers, single‐walled carbon nanotubes (SWNTs) and silica nanoparticles (SiO₂). Both SWNTs and SiO₂ were engineered specifically to become phase‐designated reinforcing functional materials, SWNT‐g‐PEG and SiO₂‐g‐HBFP, which (1) improved the dispersion of fillers, nanotubes, or spherical nanoparticles in the amphiphilic matrices, (2) enhanced the non‐covalent interactions between nanofillers and polymers, and more importantly, (3) maintained reactive functionalities to be further covalently integrated into the complex networks. Tensile moduli (E_dry) for these as‐prepared SWNT‐containing composites increased by up to 430% relative to the unfilled material, while those incorporated with SiO₂ had a 420% increase of E_dry. After swelling in water, the water absorption within the micro‐ and nanochannels of PEG‐rich domains rigidified or softened the entire crosslinked network, as determined by the amount of PEG.