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Core–dual-shell-type hybridized nanoparticles (NPs) having Au-core/dye-doped silica inner shell/Au outer shell are successfully fabricated by developing a biphasic process that is a kind of so-called “one-pot” method. The resulting hybridized NPs exhibit evidently about 20-fold enhancement of fluorescence intensity, increase in fluorescence quantum yield, and decrease in fluorescence lifetime. These effects depend on the metal nanostructure being optimized, compared with the reference hybridized NPs with neither a Au-core nor a Au outer shell, due to the gap-mode effect induced by localized surface plasmon resonance in the core–dual-shell-type MIM-like nanostructure. More detailed elucidation concerning the enhancement mechanism will provide the possibility of photonic device application, for example as a high-performance point light source, nanolaser, or sensor for bioimaging in the visible region in the near future.