Advanced technologies that can mimic hierarchical architectures found in nature can provide pivotal clues for elucidating numerous biological mechanisms. Herein, a novel technology, spontaneous organization of numerous-layer generation by electrospray (SpONGE), was developed to create self-assembled and multilayered fibrous structures. The simple inclusion of salts in a polymer solution prior to electrospraying was key to mediating the structural versatilities of the fibrous structures. The SpONGE matrix demonstrated great potential as a crucial building block capable of inducing sequential, localized drug delivery or orchestrating cellular distribution in vivo, thereby expanding its scope of use to cover a variety of biomedical applications. Multilayered, self-assembled, and volume-expanded nanofibrous structures can be formulated by a novel process referred to as the spontaneous organization of numerous-layer generation by electrospray (SpONGE). The SpONGE matrix possesses the unique ability to split multiple individual fibrous layers by manual separation and spatially position biomolecules.
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