Cellulose, an abundant natural polysaccharide, can be applied to immobilize particles on the surface due to the presence of ample hydroxyl groups. A series of different sizes and contents of gold nanoparticles (AuNP) were prepared on cellulose nanocrystal (CNC). The obtained AuNP/CNC nanocomposites were then blended with shape-memory polyurethane (SMP) to prepare light-triggered AuNP/CNC/SMP nanocomposites through solvent conversion and a solution casting method. The nanocomposite films were endowed with higher mechanical properties and striking remote-control light-triggered shape-memory properties. Moreover, the CNC in the composites also enhanced the photothermal effect of AuNPs by preventing the aggregation of AuNPs. At the same time, the content of AuNPs with existing CNC had a stronger effect on the elevated temperature (∆T) and the shape-memory properties of films in comparison to the size of the AuNPs.