Silk fibroin is widely believed to be sustainable, biocompatible,
and biodegradable, providing promising features such as carriers to
deliver drugs and functional ingredients in food, personal care, and
biomedical areas, which are consistent with emulsion characteristics;
especially, green, all-natural biopolymer-based stabilizers are in
great demand to stabilize Pickering emulsions and match the multifunctional
needs for developing ideal materials. Herein, an unprecedented three-dimensional
(3D) nanostructure, namely a brush-like silk nanobrush (SNB), is applied
as the stabilizer to formulate and stabilize Pickering emulsions.
The size and interfacial tension are compared among the SNB, a regenerated
silk nanofiber, and a nanowhisker. Additionally, optimization processes
are conducted to determine the ideal ultrasonication intensity and
SNB concentration required to prepare Pickering emulsions by analyzing
the morphology, creaming index, mean oil droplet size, and rheological
behavior. The results indicate that an SNB with the characteristic
structure and suitable size shows superior potential to form sophisticated
and interconnected networks in oil-water interfaces, and is proved
to be able to resist creaming at a wide range of concentrations and
subsequently stabilize Pickering emulsions from liquid-like emulsions
to gel-like emulsions. Additionally, SNB is proved to be biocompatible
according to cell experiments, providing a promising alternative in
designing all-natural, green, and biocompatible emulsions with the
aim of efficiently delivering nutrients or drugs associated with health
benefits.