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. Layers of vermiculite exfoliated using a new energy and time efficient method were used here as a model clay system. GO was synthesized following the modified Hummers' method. Stripes of clay–GO bilayer membranes can sense the presence of solvent molecules such as methanol, ethanol, isopropanol, tetrahydrofuran (THF), ethyl acetate, dichloromethane (DCM), acetone and water and respond to their presence by altering their own shapes in specific manners. Remarkably, stripes of bilayer membranes can unambiguously distinguish between methanol and ethanol vapors and respond to their presence by bending in opposite directions. Among the solvents tested, isopropanol induced a maximum bending speed of 1.44 degrees per second. Studies on permeability, effects of solvents on the bending stiffness and interlayer spacing of GO and vermiculite membranes provided valuable insight into the mechanism of responsive behavior. Unparalleled change in the stiffness of GO and vermiculite sections of the stripes upon exposure to solvent vapors is believed to be the driving force behind the responsiveness.