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In this paper, a new scheme for generating a wide gamut of structural colors on the thin‐film‐stack‐based (TFSB) substrates is proposed. The TFSB surfaces consist of titanium/random gold nanoparticles (AuNPs) and titanium/ random gold and copper nanoparticles (Au+CuNPs), which can trigger more resonance absorption and widen the color gamut. The electric fields in two designed structures are simulated, and the results showed that the random distribution of AuNPs and Au+CuNPs enhance the uniform local surface plasmon resonance (LSPR) response. This enhancement is crucial in broadening the coverage of the reflection spectrum, which enables the generation of a wide range of colors, including green and red. The influence of laser parameters on the color of TFSB substrates and tested their durability in terms of time is analyzed. Finally, a color palette and made structural color patterns on TFSB by nanosecond pulsed laser are prepared. The proposed new scheme can be easily fabricated by magnetron sputtering without requiring additional procedures, which can open new perspectives in plasmonic colors. This work demonstrates that the promising potential of methods in creating a wide color gamut on metallic surfaces. Additionally, it serves as a means to store information for the preservation and protection of traditional cultures. [ABSTRACT FROM AUTHOR]