This study evaluated acrylamide (AA) levels and various quality parameters in homemade fried potatoes prepared in different sizes by integrating principles from the Slow Food Movement with advanced sensor technology. To this aim, a surface plasmon resonance (SPR) sensor based on a molecularly imprinted polymer (MIP) was first developed for the determination of AA in homemade fried potatoes at low levels, and the AA levels in the samples were established. First of all, monolayer formation of allyl mercaptane on the SPR chip surface was carried out to form double bonds that could polymerize on the chip surface. AA-imprinted SPR chip surfaces modified with allyl mercaptane were prepared via UV polymerization using ethylene glycol dimethacrylate (EGDMA) as a cross-linker, N,N′-azobisisobutyronitrile (AIBN) as an initiator, and methacryloylamidoglutamicacid (MAGA) as a monomer. The prepared AA-imprinted and nonimprinted surfaces were characterized by atomic force microscopy (AFM) and Fourier transform infrared (FTIR) spectroscopy methods. The SPR sensor indicated linearity in the range of 1.0 × 10−9–5.0 × 10−8 M with a detection limit (LOD) of 3.0 × 10−10 M in homemade fried potatoes, and the SPR sensor demonstrated high selectivity and repeatability in terms of AA detection. Additionally, the highest AA level was observed in the potato sample belonging to the T1 group, at 15.37 nM (p < 0.05), and a strong and positive correlation was found between AA levels and sensory parameters, the a* value, the ΔE value, and the browning index (BI) (p < 0.05).