Recently, graphene and related materials, which exhibit enticing physical/chemical properties such as high electrical conductivity, transparency, biocompatibility, mechanical flexibility, strength, and good stability, have revealed great superiority for the development of stimuli-responsive multilayer structures toward future use in smart sensors or intelligent robots. However, complex processing procedures restrict its further applications. We reported here a facile and cost-effective preparation of moisture-responsive graphene bilayer paper by focused sunlight irradiation. The smart graphene paper shows moisture-responsive properties due to selective adsorption of water molecules, leading to controllable actuation under humid conditions. In this way, graphene-based moisture-responsive actuators including a smart claw, an orientable transporter, and a crawler paper robot have been successfully developed. This work was published in Adv. Mater. DOI: 10.1002/adma.201403587 as a cover article. Additionally, the paper has been highlighted by Nature doi:10.1038/514539d entitled “Sunshine drives graphene machines”.