Cascaded optical field enhancement (CFE) can be realized in some specially designed multiscale plasmonic nanostructures, in which the generation of extremely strong fields at nanoscale volume is crucial for many applications, for example, surface-enhanced Raman spectroscopy (SERS). In this paper, we propose a strategy for realizing a high-quality plasmonic nanoparticle-in-cavity (PIC) nanoantenna array, in which strong coupling between a nanoparticle (NP) dark mode with a high-order nanocavity bright mode can produce strong Fano resonance at the target wavelength. The Fano resonance can effectively boost the CFE in a PIC. A cost-effective and reliable nanofabrication method is developed using room temperature nanoimprinting lithography to manufacture high-quality PIC arrays. This technique guarantees the generation of only one gold NP at the bottom of each nanocavity, which is crucial for the generation of the expected CFE. To demonstrate the performance and application of the PIC array, the PIC array is employed as an active SERS substrate for detecting 4-aminothiophenol molecules. An experimental SERS enhancement factor of 2 3 10 7 is obtained, which verifies the field enhancement and the potential of this device. 1,2 SPs can be considered to be the resonant photon-induced collective oscillations of free electrons confined on the surfaces of metallic nanostructures, which can be driven by an incident light field. The importance of these photonelectron interactions is their ability to concentrate light energy in nanoscale volumes in the metallic nanostructures and subsequently boost the intensity of the optical near field by several orders of magnitude.2-5 Due to these properties, localized SPs can facilitate many applications based on the enhanced light-matter interaction, such as the detection of trace element chemical varieties in the vicinity of metallic nanostructures by surface-enhanced Raman spectroscopy (SERS). The detection limit can be reduced to a single molecular level.