water splitting, [14] and biomedical diagnosis. [15] Among many of these designs, nanoparticle-in-void structure appears more attractive as it has a uniform hemispherical gap between the nanoparticle and the inner wall of the void, promising a much higher SERS enhancement and uniformity. [16,17] However, such a nanoscale hemispherical configuration with good uniformity poses great challenge to the traditional fabrication methods. Although drop-casting of nanoparticles and thermal dewetting of the metal films in ordered porous template can produce particles in the void, their morphology is not welldefined with lots of local defects. [18][19][20][21][22][23] The gap formed via electrochemical growth appears more uniform and controllable, [24] but the gap between the particle and the inner wall of nanobowl is fully filled, which has to resort to overcoating of another Ag films to boost its SERS performance. [25] Moreover, none of these structures are dynamically tunable, making it much less versatile.Ideally, the geometry of single Au nanoparticle in bowl (Au NPiB) with a proper space in between is desired to support plasmonic hot spots for SERS, which requires 1) matchable sizes between the Au nanovoids and the Au nanoparticles (AuNPs); 2) properly functionalized surfaces that hinder the aggregation of AuNPs during the assembly process; 3) monolayer of AuNPs to avoid random stacking. It is nontrivial to meet all these three requirements although it is quite easy to achieve one or two via conventional self-assembly or colloidal lithography.Here, we employ anodic aluminum oxide (AAO) as the nanobowl template, which are sputter-coated with Au films to generate Au nanobowl arrays. The size of these nanobowls is ≈80 nm which is slightly larger than the AuNPs (≈60 nm) used for self-assembly (Requirement 1). These AuNPs are coated with poly(N-isopropylamide) (PNIPAM), which not only provides steric hindrance against aggregation but also endows the thermal tunability of the plasmonic system (Requirement 2). The Au@PNIPAM NP monolayer assembled at liquidliquid interface is transferred to the Au nanobowl arrays via dip-coating so that each void of nanobowl is filled with just one Au@PNIPAM NP (Requirement 3). As the gap between the AuNP and the Au bowl is filled with PNIPAM, their separation can be reversibly tuned by simply controlling the Plasmonic nanoresonators made of particle-in-void have been considered as superior plasmonic cavities for surface enhanced Raman scattering (SERS). However, controlled fabrication of such plasmonic system and its dynamic tuning pose great challenges to traditional fabrication methods. Here, a capillary-driven self-assembly is proposed to form gold nanoparticles in bowls (Au NPiBs), which have a nm-gap filled with temperature-responsive polymers (poly(N-isopropylacrylamide)). As such, the plasmonic resonances of the Au NPiB nanostructures can be dynamically and reversibly tuned with the change of temperature due to the thermally induced expansion and contraction of the polymers. The SERS e...