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As one of the important materials, nanocrystalline Au (n-Au) has gained numerous interests in recent decades owing to its unique properties and promising applications. However, most of the current n-Au thin films are supported on substrates, limiting the study on their mechanical properties and applications. Therefore, it is urgently desired to develop a new strategy to prepare n-Au materials with superior mechanical strength and hardness. Here, a hard n-Au material with an average grain size of ∼ 40 nm is prepared by cold-forging of the unique Au nanoribbons (NRBs) with unconventional 4H phase under high pressure. Systematic characterizations reveal the phase transformation from 4H to face-centered cubic (fcc) phase during the cold compression. Impressively, the compressive yield strength and Vickers hardness (HV) of the prepared n-Au material reach ∼ 140.2 MPa and ∼ 1.0 GPa, which are 4.2 and 2.2 times of the microcrystalline Au foil, respectively. This work demonstrates that the combination of high-pressure cold-forging and the in-situ 4H-to-fcc phase transformation can effectively inhibit the grain growth in the obtained n-Au materials, leading to the formation of novel hard n-Au materials. Our strategy opens up a new avenue for the preparation of nanocrystalline metals with superior mechanical property. [Figure not available: see fulltext.]. © 2022, Tsinghua University Press.