Clay nanosheets (CNSs) have been widely used in the design of nanocomposite biomaterials. CNSs display a disk-like morphology with strong negatively charged surfaces. It has been shown that guanidinium-containing molecules can bind CNSs through noncovalent salt-bridge interactions and thus serve as "molecular glues" for CNSs. Making use of the guanidinium side chain in arginine, here, we designed novel arginine-rich elastomeric proteins to engineer protein-CNS nanocomposite hydrogels. Our results showed that these arginine-rich proteins can interact with CNSs effectively and can cross-link CNSs into hydrogels. Rheological measurements showed that mechanical properties of the resultant hydrogels depended on the arginine content in the arginine-rich proteins as well as CNS/protein concentration. Compared with hydrogels constructed from CNSs or proteins alone, the novel protein-CNS nanocomposite hydrogels show much improved mechanical properties. Our work opens up a new avenue to engineer functional protein hydrogels for various applications.