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The present study aimed to improve the optical sensing performance of tapered optical fiber sensors toward aqueous Rhodamine B solution of different concentrations by applying single-walled carbon nanotubes (SWCNTs). The functional coating was formed on the surface of the tapered optical fiber sensor using an aerosol layer-by-layer deposition method. Before deposition, the SWCNTs were processed with multistage liquid-phase treatment in order to form a stable dispersion. The effect of SWCNT treatment was investigated through Raman spectroscopy. The deposition of 220 layers caused a reduction of up to 60% of the initial optical power of radiation propagating through the optical fiber core. The optical fiber sensor coated with SWCNTs demonstrated significantly higher sensitivity compared to a non-coated sensor in the range of 2–32 mg/L of Rhodamine B concentration in an aqueous solution. The experimental results demonstrated that the sensitivity was increased 10 times from 32 (mg/L)⁻¹, for the non-coated sensor, up to 317 (mg/L)⁻¹ after SWCNT coating deposition. Moreover, the SWCNT-coated sensor demonstrated high repeatability that allowed for the evaluation of the concentration regardless of the previously analyzed dye concentration.