a large surface to volume ratio [7] ) and have broad applications (e.g., energy conversion, [8] smart robots, [9] and biomedical devices [10] ). Recently, Ariga and co-workers achieved highly selective gas sensing using ionic liquid-intercalated graphene layers that were prepared by in situ reduction of graphene oxide layers in the presence of nonvolatile ionic liquids, and subsequent electrostatic layer-by-layer assembly. [11] Sadasivuni et al. presented the layer-bylayer spraying of modified graphene oxidefilled cellulose nanocrystals for proximity sensing. [12] Wang et al. reported ultrathin reduced graphene oxide (RGO) films with controllable thicknesses for noncontact relative humidity (RH) sensing. [13] In our previous works, an RGO with hierarchical micro-nanostructures prepared by two-beam-laser interference was employed to produce humidity-sensing devices. [14] However, in spite of these advancements, graphene-based sensing devices have not been well employed for smart device design. A possible reason for this gap would be the difficulty in tailoring highly permeable graphene nanostructures that permit spontaneous, timely, and reliable molecular discrimination. Moreover, complex experimental procedures or special instruments are generally necessary in device fabrication, which largely limits their integration with other devices. The current trend is to produce smart devices equipped with versatile sensors created in facile, reliable, cost-effective, and environmentally friendly manners. However, it is currently challenging to achieve this goal.Herein, we report a facile preparation of a graphene-based moisture detector for smart device design. A humidity-sensing device has been fabricated by a simple focused sunlight treatment of GO. The drastic removal of oxygen-containing groups (OCGs) not only mediates the controllable tuning of conductive properties but also leads to the formation of a highly porous RGO structure that is of benefit to the adsorption of molecules and humidity sensitivity. The RGO-based humidity-sensing device shows moisture recognition capability and excellent sensing performance, including high sensitivity, good repeatability, small humidity hysteresis, and fast response recovery at room temperature, enabling a series of humidity-sensing devices including a moisture controller, a humidity detector robot, and even a novel electronic harmonica. As a simple and chemical-free method, sunlight-mediated photoreduction of GO provides a very simple and cost-effective way to integrate humidity sensors in the development of versatile moistureresponsive smart devices.Here, a facile fabrication of graphene-based humidity sensors is reported for smart device design. Focused sunlight photoreduction of graphene oxide (GO) helps to remove most of the oxygen-containing groups on GO sheets, which not only recovers their conductivity but also leads to the formation of a highly porous nanostructure, enabling the manufacture of versatile humidity-sensing smart devices, such as moisture controllers, hu...