PEI)-assisted crosslinking with catechol moieties, which could further be used as a Janus platform to support the reduction and attachment of silver nanoparticles on the film surface. [7] Freestanding organicmetal 2D films have potential in many application fields, such as in sensing, surface-enhanced Raman scattering, catalytic reaction, near-infrared photothermal therapy, and biomedical areas. [8][9][10][11] Unfortunately, such films are fabricated via multiple, time-consuming steps; [11,12] in addition, the sacrifice of metal conductivity greatly limits the applications of these materials in the electrical device field. [2,13] Herein, we report a facile, environmentally friendly and bio-based redox system to merge metal nanoparticles under ambient conditions in an aqueous solution via protein bonding, which is distinctive from traditional welding of nanomaterials at high temperatures/ pressures. We discover that the silver nanoparticles from the in situ reduction of silver ammonium ions by glucose were bound by ultrathin amyloid-like β-sheet stacking of lysozyme to create a freestanding large-area (e.g., 400 cm 2 ) 2D silver film at the air/water interface with a purity up to 98%. We prove the great ability of this reaction system toward controlled synthesis of highly reflective and highly conductive silver films with elongation nearly 10 times higher than that of pure metal without protein bonding. These characteristics allow the protein-bound silver films to crucially participate in realistic applications, such as in strain/pressure sensors and artificial throats with ultrasensitive capability for stealth transmission of Morse code via the detection of minute finger tapping and for silent speech recording via the detection of tiny vibrations of the human throat, a result never reported before. No special equipment is necessary for this one-step method, and we further demonstrate that the bonding function of lysozyme is general to other proteins (e.g., albumin, α-amylase, collagen, keratin, and pepsin) and other metal films besides Ag (e.g., Au and Cu) are synthesized easily by this strategy.The protein assembler lysozyme, generally recognized as a safe material by the US Food and Drug Administration, is commercially available at low cost from egg white, body fluids of animals and plant cells. [14] Figure 1a schematically illustrates the synthetic procedures of a lysozyme-bound silver film. Lysozyme from egg white, Tollen's reagent, and d-glucoseThe welding and sintering of nanomaterials is usually achieved at high temperatures and high pressures. Here, it is found that merging of metal nanoparticles occurs under ambient conditions in an aqueous solution via protein bonding. It is discovered that the silver nanoparticles from the in situ reduction of silver ammonium ions by glucose undergo confined nucleation and growth and are bound by ultrathin amyloid-like β-sheet stacking of lysozyme. This merging of silver nanoparticles creates a freestanding large-area (e.g., 400 cm 2 ) 2D silver film at the air/water i...