Nanofibrillated bacterial cellulose (NFBC), a type of cellulose nanofiber biosynthesized by Gluconacetobacter sp., has extremely long (i.e., high-aspect-ratio) fibers that are expected to be useful as nanofillers for fiber-reinforced composite resins. In this study, we investigated a composite of NFBC and poly(methyl methacrylate) (PMMA), a highly transparent resin, with the aim of improving the mechanical properties of the latter. The abundant hydroxyl groups on the NFBC surface were silylated using 3-(methacryloyloxy)propyltrimethoxysilane (MPTMS), a silane coupling agent bearing a methacryloyl group as the organic functional group. The surface-modified NFBC was homogeneously dispersed in chloroform, mixed with neat PMMA, and converted into PMMA composites using a simple solvent-casting method. The tensile strength and Young’s modulus of the composite increased by factors of 1.6 and 1.8, respectively, when only 0.10 wt% of the surface-modified NFBC was added, without sacrificing the maximum elongation rate. In addition, the composite maintained the high transparency of PMMA, highlighting that the addition of MPTMS-modified NFBC easily reinforce PMMA. Furthermore, interactions involving the organic functional groups of MPTMS were found to be very important for reinforcing PMMA.