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Modulating surface wrinkling is important for a variety of engineering applications. It has been known for more than two decades that the wavelength of surface wrinkles occurring in a metal film–soft polymer system scales linearly with the deposited film thickness. In the current experimental study of ultrathin gold film (0.2–8 nm) deposition on polydimethylsiloxane (PDMS), an unexplored thickness-dependent wrinkling phenomenon is found. By manipulating the deposition sequence as a degree of freedom for tailoring surface topography, we discovered a morphology memory effect where the wrinkle evolution in the subsequent deposition step inherits the surface pattern already formed in the previous step. Moreover, a stepwise deposition targeting 1 nm thick film can lead to 1 order of magnitude higher surface roughness than the one in the continuous deposition. By programming the sequences within 8 nm Au …