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The well-known integration of outstanding optical, electronic, and catalytic properties enables Au nanomaterials to be applied in various fields, however, the intrinsically easy plastic flow of Au nanomaterials results in insufficient mechanical durability. Herein, the strategy of assembling core-shell structure to enclose Au nanoparticles is presented to tune the mechanical response for enhancing durability. Under the impact of the catalytic property of Au nanoparticles, the unique nanoshell containing the curved fullerene-like carbon (FL-C) fragments and amorphous carbon (a-C) tissue can self-assemble around Au nanoparticles and encapsulate adjacent Au nanocores, forming the Au@a-C/FL-C core-shell structure via co-sputtering method. Compared to pure Au film, such self-assemble Au@a-C/FL-C film can transform the mechanical response from plastic flow to the desirable near-elastic response. Additionally, the novel Au@a-C/FL-C structure also endows favorable properties such as high strength (∼13.7 GPa), high elastic recovery (∼90%), and low wear rate (1.51 × 10−7 mm3/Nm), which are even superior to the traditionally considered protective-lubricating a-C film. The structural characteristic of Au@a-C/FL-C film can provide a route to design Au-based materials with enhanced strength, near-elastic response, and high durability for resisting wear.
•The ultra-thin carbon cages containing FLC fragments and a-C components can uniformly encapsulate Au nanoparticles.•The Au@a-C/FL-C structure leads elastic recovery ramping to 90%, which successfully delaying the onset of plastic flow.•The Au@a-C/FL-C film yields thecombinations of the high hardness, high elastic recovery, and the ultra-low wear rate.