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Flexible membrane consisting of ultralong VO@conducting polypyrrole (VO@PPy) core-shell nanowires is prepared by a facile in situ interfacial synthesis approach. The VO is for the first time demonstrated to show versatile function of reactive template to initiate the uniform and conformal polymerization of PPy nanocoating without the need for extra oxidants. The freestanding PPy-encapsulated VO nanowire membrane is of great benefit in achieving strong electrochemical harvest by increasing electrical conductivity, shortening ion/electron transport distance, and enlarging electrode/electrolyte contact area. When evaluated as binder- and additive-free supercapacitor electrodes, the VO@PPy core-shell hybrid delivers a significantly enhanced specific capacitance of 334 F g along with superior rate capability and improved cycling stability. The present work would provide a simple yet powerful interfacial strategy for elaborate constructing VO/conducting polymers toward various energy-storage technologies.

Three-dimensional (3D) microfibrillar network represents an important structural design for various natural tissues and synthetic aerogels. Despite extensive efforts, achieving high mechanical properties for synthetic 3D microfibrillar networks remains challenging. Here, we report ultrastrong polymeric aerogels involving self-assembled 3D networks of aramid nanofiber composites. The interactions between the nanoscale constituents lead to assembled networks with high nodal connectivity and strong crosslinking between fibrils. As revealed by theoretical simulations of 3D networks, these features at fibrillar joints may lead to an enhancement of macroscopic mechanical properties by orders of magnitude even with a constant level of solid content. Indeed, the polymeric aerogels achieved both high specific tensile modulus of ~625.3 MPa cm3 g−1 and fracture energy of ~4700 J m−2, which are advantageous for diverse structural applications. Furthermore, their simple processing techniques allow fabrication into various functional devices, such as wearable electronics, thermal stealth, and filtration membranes. The mechanistic insights and manufacturability provided by these robust microfibrillar aerogels may create further opportunities for materials design and technological innovation.