This article presents a detailed study on the nanoscaled interface between microelongated gold particles (GP) and biphase leucite/feldspar glass-ceramic matrix. The glass-ceramic composite with a nonuniform GP distribution was processed through hot-pressing under vacuum using a commercial dental ceramic furnace for glass-ceramic dental crown manufacturing. Heat treatments at 900°C, 1100°C, and 1300°C were conducted, and microstructural features along the interface were used to verify the chemical reactions between GP and glass-ceramic matrix. It was observed that the amorphous glass-ceramic matrix had nanoscaled biphase structures, and the distributed nanoscaled amorphous leucite phase was attracted to GP during hot-pressing, and was more reactive with GP than the feldspar phase. The thickness of the interfacial phase formed through chemical reactions between GP and glass-ceramic matrix is around 30 nm. The chemically bonded interface has contributed significantly toward the substantial improvements in both strength and toughness of the GP-reinforced glass-ceramic matrix composite. Characterization techniques, including X-ray diffraction and field-emission scanning electron Microscopy, incorporating X-ray microanalysis using energy dispersive spectrometry, have been employed in this study.