The feasibility of a localized surface plasmon resonance (LSPR) enhanced sensor based on raspberry-like nanosphere functionalized silica microfibers has been proposed and experimentally demonstrated. The extinction of single Ag (or Au) nanoparticles usually occurs at visible wavelengths. Nevertheless, a LSPR enhancement at near infrared wavelengths has been achieved by constructing raspberry-like meso-SiO₂ nanospheres with noble metal nanoparticle cluster coating. The nanosphere coating captures γ-amino-butyric acid (GABA) targets through size selectivity and enhances the sensitivity by the LSPR effect. The gathering of GABA on the sensor surface translates the concentration signal to the information of refractive index (RI). Silica microfiber perceives the RI change and translates it to optical signal. The LSPR effect enhances the optical sensitivity by enhancing the evanescent field on the microfiber surface. This combination presents the lowest limit of detection (LOD) of 10⁻¹⁵ M (three orders lower than that without LSPR enhancement). It could fully afford the detection of ultra-low GABA concentration fluctuation (which is important for determining a variety of neurological and psychiatric disorders). The inherent advantages of the proposed sensors, including their ultra-sensitivity, low cost, light weight, small size and remote operation ability, provide the potential to fully incorporate them into various biomedical applications.