The objective of this study was to develop a novel resin composite containing yttrium aluminum garnet (Y3Al5O12, YAG) nanoparticles for clear aligner attachments. After the silanization of YAG, their Fourier-transform infrared (FT-IR) and thermogravimetric (TGA) analyses were performed. By conducting flexural and compressive strength measurements, the optimal YAG concentration was selected for the subsequent experiments. Next, Vickers microhardness values, fluidities, attachment volumes, conversion degrees, and volumetric shrinkages of the resin were determined. The obtained FT-IR and TG results revealed that γ-methacryloxypropy ltrimethoxysilane coupling agent was successfully grafted onto the surface of YAG, which enabled their use as inorganic fillers. Furthermore, adding 9 wt% YAG in the resin can increase Vickers hardness and fluidity, reduce polymerization shrinkage, and enhance the restoration of the clear aligner attachment shape on the premise of guarantee proper flexural and compressive strength of the resin, which can help control tooth movement and increase orthodontic efficiency.