Layers of naturally occurring clay minerals are rearranged to prepare highly sensitive multiresponsive clay-clay bilayer membrane (CCBM). The CCBM introduced here responds to the minuscule changes in the surrounding environments including temperature, humidity, and presence of solvent vapors by morphing in specific manners. Strips cut from CCBM exhibit up to 588 N kg force output when exposed to temperature fluctuations. Inheriting the natural stability of clay minerals, CCBM demonstrates extreme robustness, heating up to 500 °C, cooling with liquid N and exposure to corrosive chemical vapors did not deteriorate its bending performance. Mechanistic studies suggest that shape transformations of CCBM are driven by the unequal response of its components to external stimuli.

The reactive surface and layered crystal structure of vanadium pentoxide (V2O5) are exploited here to prepare a two-dimensional (2D) ion pump that transports ions against their concentration gradient.

Bilayer membranes that can morph in a controlled manner were prepared by restacking exfoliated layers of clay and graphene oxide (GO) from their respective aqueous dispersions.

Owing to their abundance, ecofriendliness, and multifaceted properties, natural clay minerals are among the most trusted and widely utilized materials on earth. One of the most exciting and latest findings of these minerals is that their layers can be exfoliated into individual flakes and reassembled to produce freestanding and flexible membranes. A tremendous surge in the research related to the futuristic applications of lamellar membranes prepared by restacking exfoliated two-dimensional (2D) nanomaterials has been observed in recent years. In this review article, we aim to summarize the multidirectional progress of lamellar membranes prepared from natural clay minerals. Innovative strategies involved in the exfoliation of clay layers and fabrication of macroscopic membranes through various assembly techniques are highlighted with special emphasis on novel applications such as studying nanofluidic transport in strict 2D, fabrication of smart materials, carrying out chemical reactions under nanoscale confinement, harvesting blue energy, and molecular separation. The clay membranes also inherit extraordinary robustness from their parent minerals and hence open up novel avenues for unique combinations of delicate properties and extraordinary thermal and chemical stability such as hightemperature stable ionic conductors, thermally stable smart materials, and high-temperature energy devices. Exceptional properties imbued to natural clay minerals such as tunable surface wettability and water-assisted healing of physical damage and functional properties by exchanging their inherent interlayer cations are also discussed elaborately.

The balance between expanding and contracting forces of lamellar clay minerals was exploited for preparing self-repairable nanofluidic membranes.