In recent years, the authors have been developing novel fluoride-releasing dental composites containing ternary zirconium fluoride chelates. The aim of this study was to improve the physical and mechanical properties of these composites by improving the formulation of the monomers and photoinitiators. The hypothesis was that reduction of hydrophilic monomers and improvement of the photoinitiators could reduce water sorption and significantly increase the mechanical properties of the composite. The degree of conversion of the composites containing different compositions of photoinitiators was studied by Fourier transform near-infrared spectroscopy (FT-NIR). Ten experimental composites containing different compositions of ethoxylated bisphenol-A dimethacrylate (EBPADMA), 1,6-hexanediol dimethacrylate (HDDMA), triethylene glycol dimethacrylate (TEGDMA), and 2,2-bis[4-(2-hydroxy-3-methacryloyloxypropoxy)phenyl]-propane (BisGMA) were tested for flexural strength, viscosity, and water sorption. The experimental composite containing 20% synthesized fluoride-releasing monomer, 30% BisGMA, 30% EBPADMA, and 20% HDDMA showed significantly higher fluoride release and recharge, but physical and mechanical properties similar to those of the control composite containing 40% BisGMA, 40% EBPADMA, and 20% HDDMA.