Graphene polymers-based soft actuators driven by infrared (IR) light have attracted wide attention recently. However, the scientific fraternity is striving hard in unraveling the area of actuators that could be triggered by IR light along with chemicals. The fabricating methodology of multiresponsive soft actuators based on graphene nanoplatelets (GNPs)-poly(dimethylsiloxane) (PDMS) nanocomposite/gold bilayers, ensuring large, fast, and reversible response, has been illustrated. The actuators display a novel dual-mode operation as photomechanical and chemomechanical actuation. The actuators are realized by depositing a thin film (100 nm) of gold on GNP-PDMS nanocomposite films resulting tubular structure on account of thermal residual stress. The actuation response of this structure upon its exposure to IR light and chemicals was measured in terms of percentage opening and degree of unscroll, respectively. The three-dimensional tubular structure is transformed into a two-dimensional sheet within 8 s under IR light irradiation. The same structures were also tested in various organic solvents like methanol, ethanol, acetone, isopropyl alcohol, and aldehydes, but the actuation has been observed only in acetone and aldehydes. This tubular actuator unscrolls completely and then scrolls in opposite direction along with tube axis shift through 90° during its exposure to acetone (liquid/vapors) and aldehydes. Few applications of these actuators, such as multimode soft grippers for on-demand capture/release of objects (with weight 1.2 times the actuator's own weight) and volatile organic compounds detection module, have been demonstrated. The combination of surface micromachining techniques of microelectromechanical systems process with this smart material may find applications in drug-delivery systems with precise control, soft robotics, and noninvasive diagnosis of diabetes and breast/lung cancers.