We report on the measurement of the response of Rhodamine 6G (R6G) dye to enhanced local surface plasmon resonance (LSPR) using a plasmonic-active nanostructured thin gold film (PANTF) sensor. This sensor features an active area of approximately ≈ 2.5 × 10¹³ nm² and is immobilized with gold nanourchins (GNU) on a thin gold film substrate (TGFS). The hexane-functionalized TGFS was immobilized with a 90 nm diameter GNU via the strong sulfhydryl group (SH) thiol bond and excited by a 637 nm Raman probe. To collect both Raman and SERS spectra, 10 μL of R6G was used at concentrations of 1 μM (6 × 10¹² molecules) and 10 mM (600 × 10¹⁴ molecules), respectively. FT-NIR showed a higher reflectivity of PANTF than TGFS. SERS was performed three times at three different laser powers for TGFS and PANTF with R6G. Two PANTF substrates were prepared at different GNU incubation times of 10 and 60 min for the purpose of comparison. The code for processing the data was written in Python. The data was filtered using the filtfilt filter from scipy.signals, and baseline corrected using the Improved Asymmetric Least Squares (ISALS) function from the pybaselines.Whittaker library. The results were then normalized using the minmax_scale function from sklearn.preprocessing. Atomic force microscopy (AFM) was used to capture the topography of the substrates. Signals exhibited a stochastic fluctuation in intensity and shape. An average corresponding enhancement factor (EF) of 0.3 × 10⁵ and 0.14 × 10⁵ was determinedforPANTFincubated at 10 and 60 min, respectively.