The graphene nanosheets (GNS)/polydimethylsiloxane (PDMS) composite films with out-of-plane dielectric actuation behavior were prepared through a layer-by-layer spin coating process. The GNS-PDMS/PDMS composite films with 1~3 layers of GNS-PDMS films were spin coated on top of the PDMS film. The dielectric, mechanical, and electromechanical actuation properties of the composite films were investigated. The dielectric constant of the GNS-PDMS3/PDMS composite film at 1 kHz is 5.52, which is 1.7 times that of the GNS-PDMS1/PDMS composite film. The actuated displacement of the GNS-PDMS/PDMS composite films is greatly enhanced by increasing the number of GNS-PDMS layers. This study provides a novel alternative approach for fabricating high-performance actuators with out-of-plane actuation behavior.