Molar pits and fissures tend to be affected by caries due to cleaning difficulties. As such, the filling of pits and cracks with sealants is common to deter the onset of caries. However, current clinical practices rely on sealants that lack the ability to release and recharge fluoride ions. Thus, we herein report the development of a fluoride-montmorillonite nanocomposite resin that has the potential to provide sustained release of fluoride due to the strong adsorption of fluoride by montmorillonite. X-ray diffractometry, thermogravimetric analysis, and Fourier-transform infrared spectroscopy were employed to confirm the successful insertion of the polymer into the interlayer structure. The mechanical properties (viscosity, hardening depth, hardness, diametral tensile strength, flexural strength, and wear resistance) of the developed composite resin were then examined, and simulation of the oral environment demonstrated a good fluoride ion release and recharge ability for the effective prevention of dental caries. Finally, we demonstrated the non-cytotoxic nature of this material using the water-soluble tetrazolium salt (WST-1) test. We expect that the described fluoride-containing composite resin may become a new clinical option in the near future.