as plasmonic hot-spots. [2] The resulting spectroscopic technique, known as surface-enhanced Raman spectroscopy (SERS), [3] surpasses the inherently low sensitivity of Raman by counterbalancing its low scattering efficiency [4] through spatial localization of the sample molecules proximal to the hot-spots on SERS substrates. So far colloidal nanoparticles of various shapes and sizes have been extensively used in SERS; [5][6][7][8][9] however, the lack of control over their relative orientation and separation limits efficient plasmonic coupling therebetween. [10] While this issue is addressed in SERS substrates made of immobilized nanoparticles, [11][12][13][14] interparticle gaps in these substrates are typically optimized to generate maximum field confinement for single wavelengths. Broadband SERS substrates can be made by immobilizing a mixture of nanoparticles resonant over a range of laser wavelengths on surface plasmon polariton (SPP)-supporting thin films. [15,16] However, the magnitude of SERS signal enhancement and the broadband nature of such substrates remain highly dependent on the nanoparticle-film separation as well as the interparticle distances which are difficult to control in practice. More robust broadband SERS substrates have been recently fabricated by sputtering randomly sized silver nanoparticles on glass-silver-glass multilayered substrates, [17] yielding plasmonic resonances over the 400-1100 nm