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Carbon‐based materials are widely used as light‐driven soft actuators relying on their thermal desorption or expansion. However, applying a passive layer in such film construction greatly limits the actuating efficiency, e.g., bending amplitude and speed. In this work, a dual active layer strengthened bilayer composite film made of graphene oxide (GO)–polydopamine (PDA)–gold nanoparticles (Au NPs)/polydimethylsiloxane (PDMS) is developed. In this film, the conventional passive layer is replaced by another AuNPs‐enhanced thermal responsive layer. When applying NIR light exposure, the whole film deforms controllably resulting from the water loss in the GO–PDA–Au NPs layer and thermal expansion in the PDMS layer. Benefiting from the dual active bilayer mechanism, the thin film's actuating efficiency is dramatically improved compared with that of conventional methods. Specifically, the bending amplitude …