an integral part of advanced sensing technologies. [1][2][3][4][5][6][7][8][9][10] Various optical principles, such as interference, scattering, total internal reflection, and surface plasmon resonance, are applied in designing fiberoptic (FO) sensors. [11][12][13][14][15][16][17] As an emerging FO device, nanostructured plasmonic FO sensors have attracted much attention due to their superior performance and peculiar properties. [18][19][20][21][22] As nanostructured plasmonic FO sensors feature the characteristics of both traditional FO sensors and plasmonic sensors, they exhibit unique advantages and can be used as powerful biochemical sensing tools or integrated photonic devices. [23][24][25] There have been many reports on the fabrication of plasmonic FO sensors based on metal nanostructures. [26] A simple approach is the use of metal nanoparticles to modify the side or end of the fiber to excite the surface plasmon resonance effect. [27][28][29] Although such methods have the advantages of low cost and simple preparation processes, they present some difficulties in structural control during the fabrication of nanostructures on optical fiber surfaces. In addition, sensors fabricated by these methods usually operate in visible wavebands, which lack an associated communications infrastructure. To overcome these inherent weaknesses, nanoimprint lithography, electronbeam lithography, focused ion beam approaches, reactive ion etching, two-photon polymerization, optical 3D µ-printing, laser erosion direct writing, and other technologies have been proposed and applied to manufacture controllable patterns on the fiber end face. [30][31][32][33][34][35][36][37][38][39][40][41][42] However, these techniques always depend on expensive equipment, which leads to a high-cost and time-consuming production process. As alternative techniques, breath figure methodologies and nanosphere lithography have been employed to fabricate nanostructures on the optical fiber end face. [43,44] Although these methods are cost-effective and produce regular patterns, they have some potential drawbacks that need to be improved. For instance, ceramic ferrule is an essential part of the self-assembly process, which weakens the miniaturization advantage of the fiber probe. In addition, these methods still require professional operation and specialized equipment for the process steps, such as fiber polishing, spin coating, and plasma processing. In general, owing to the high cost, process complexity, and dependence on specialized equipment, hardly any ordinary laboratories fabricate plasmonic FO As an emerging and promising paradigm of nanophotonic "lab-on-a-chip" devices, plasmonic fiber-optic (FO) probes with nanopatterns suffer from high cost and a complex fabrication process, which keep them from becoming the preferred choice for most optical fiber sensing applications. In this paper, a nanopatterned FO probe is demonstrated to be a surface-enhanced Raman spectroscopy substrate and a plasmonic biosensor through theoretical simulations and exp...