The interaction of electromagnetic waves with condensed matter and the resultant force is fundamental in the physical sciences. The maximum pressure on a planar surface is understood to be twice the incident wave power density normalized by the background velocity. We demonstrate for the first time that this pressure can be exceeded by a substantial factor by structuring a surface. Experimental results for direct optomechanical deflection of a nanostructured gold film on a silicon nitride membrane illuminated by a laser beam are shown to significantly exceed those for the planar surface. This enhanced pressure can be understood as being associated with an asymmetric optical cavity array realized in the membrane film. The possible enhancement depends on the material properties and the geometrical parameters of the structured material. Such control and increase of optical pressure with nanostructured material should impact applications across the physical sciences. © 2019 American Physical Society.