Self-assembly of nanoparticles (NPs) to form structural colors offers promising opportunities for developing electronic, optoelectronic, and magnetic devices. In this regard, we reported co-assembly of cellulose nanofibrils (CNFs) and graphene to produce colored thin films. We demonstrated that biomimetic iridescent "peacock feather"-like full-color thin films can be generated by simple evaporation of aqueous suspensions on a surface tension confined, optically symmetric indium tin oxide-coated polyethylene terephthalate substrate. Amphiphilic CNFs serve dual functions to attract hydrophobic graphene via van der Waals interactions and to disperse hydrophilically and anionically CNF-tethered graphene while regulating surface tension to induce capillary and Marangoni flows in the force fields and construct thickness variation during dewetting. These CNF-graphene thin films exhibit full-color patterns and function as tunable light and moisture actuators. This approach has high potential to be applied to assemble other metal or metal oxide NPs for fast, simple, and robust fabrication without involving any complex lithography and external fields.