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Abstract Shape‐persistent, conductive ionogels where both mechanical strength and ionic conductivity are enhanced are developed using multiphase materials composed of cellulose nanocrystals and hyperbranched polymeric ionic liquids (PILs) as a mechanically strong supporting network matrix for ionic liquids with an interrupted ion‐conducting pathway. The integration of needlelike nanocrystals and PIL promotes the formation of multiple hydrogen bonding and electrostatic ionic interaction capacitance, resulting in the formation of interconnected networks capable of confining a high amount of ionic liquid (≈95 wt%) without losing its self‐sustained shape. The resulting nanoporous and robust ionogels possess outstanding mechanical strength with a high compressive elastic modulus (≈5.6 MPa), comparable to that of tough, rubbery materials. Surprisingly, these rigid materials preserve the high ionic conductivity of original ionic liquids (≈7.8 mS cm⁻¹), which are distributed within and supported by the nanocrystal network‐like rigid frame. On the one hand, such stable materials possess superior ionic conductivities in comparison to traditional solid electrolytes; on the other hand, the high compression resistance and shape‐persistence allow for easy handling in comparison to traditional fluidic electrolytes. The synergistic enhancement in ion transport and solid‐like mechanical properties afforded by these ionogel materials make them intriguing candidates for sustainable electrodeless energy storage and harvesting matrices. 

Stacking atomically thin two-dimensional (2D) nanosheet materials leads to unique synergy in their inherent properties due to an intimate combination and matching that is not possible via separate individual components and phases. However, traditional synthesis and assembly methods result in poor architectural control and restricted surface chemistry, thereby limiting their prospective potentials. This brief overview provides consideration of different synthesis and assembly methods for fabrication of diverse novel heterostructures. The advantages and challenges of existing methods are discussed. Finally, future perspectives regarding crafting of heterostructures with highly controllable architectures and interfacial/surface chemistry, and advanced characterization methods are highlighted. 

We discuss current trends in developing novel synthetic polymers, biopolymers, and corresponding soft and functional hybrid nanocomposites for advanced current and future applications with an emphasis on active functional devices and functions. Among a wide variety of polymeric materials and relevant applications, we select the fields, which are close to the authors’ research interests. This selection includes strong but lightweight biopolymer composites, gel-like and porous materials for chemical and energy transport control, fast-actuating responsive materials and structures, and thin film electronic materials for chemical, physical, and biological sensing applications compatible with human and robotic interfaces.