Nanoemulsions are a versatile means to create a variety of consumer products and complex materials. Producing nanoemulsions with a high volume fraction of the dispersed phase is generally limited to mechanically intensive processes, such as high-pressure homogenization, and often results in polydisperse droplet size distributions. Low-energy methods, such as spontaneous emulsification, can produce monodispersed droplets, but the volume fraction of the dispersed phase is usually much lower. Here, we report on the spontaneous emulsification of 3-(trimethoxysilyl) propyl methacrylate (TPM) into an alkaline aqueous phase (pH > 10.0) that contains surfactants (Tween 20, sodium dodecyl sulfate (SDS), or cetyltrimethylammonium bromide (CTAB)). The nanoemulsions are monodisperse with droplet diameters that range between 15 and 500 nm. The small droplet size is due to the presence of surfactants that stabilize the droplets against coalescence. The spontaneous emulsion process can produce emulsions with a dispersed volume fraction of up to 10% in CTAB solutions and up to 30% using Tween 20 and SDS. After the emulsification process, the TPM droplets can be polymerized to produce nanoparticles. Using dynamic light scattering and scanning electron microscopy, we characterize the relationship between the surfactant concentration and the size of the droplets in the nanoemulsions. We find that the droplet diameter is primarily determined by the molar ratio of oil to surfactant. We also find that the pH in the aqueous phase also modulates the droplet diameter when using,an ionic surfactant. This work expands the spontaneous emulsification of TPM in the absence of stabilizing particles to the nanoscale while producing one of the highest volume fractions of nanoemulsion droplets obtained via a low-energy mechanism.