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Integration of functional nanomaterials with optical micro/nanofibers (OMNFs) can bring about novel optical properties and provide a versatile platform for various sensing applications. OMNFs as the key element, however, have seldom been investigated. Here, we focus on the optimization of fiber diameter by taking micro/nanofiber-based localized surface plasmon resonance sensors as a model. We systematically study the dependence of fiber diameter on the sensing performance of such sensors. Both theoretical and experimental results show that, by reducing fiber diameter, the refractive index sensitivity can be significantly increased. Then, we demonstrate the biosensing capability of the optimized sensor for streptavidin detection and achieve a detection limit of 1 pg/mL. Furthermore, the proposed theoretical model is applicable to other nanomaterials and OMNF-based sensing schemes for performance optimization.