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Uniform lamellar silver nanoleaves (AgNLs) were spontaneously assembled from 4 nm silver nanoparticles (AgNPs) with p-aminothiophenol (PATP) as mediator under mild shaking at room temperature (RT). The compositions of the AgNLs were verified to be ~1 nm Ag25 nanoclusters and PATP molecules in quinonoid model. The underlying assembly mechanism was systematically investigated and a two-step reaction process was proposed.