In this study, hydrothermally synthesized {[Nd(SIP)(H2O)4]}n (NdSIP) and carboxylate-modified SiO2 spheres were used to obtain SiO2@NdSIP nanocomposites. Different concentrations of NdSIP in the range of 5–15%wt. were used in the hydrothermal synthesis of SiO2@NdSIP nanocomposites. NdSIP has been structurally characterized by single crystal X-ray diffraction technique. NdSIP and SiO2@NdSIP nanocomposites were characterized using various techniques including field emission scanning electron microscopy (FESEM), thermogravimetric analysis (TGA), Hirshfeld surface analysis, Fourier transform infrared (FTIR), solid-state UV absorption and photoluminescence (PL) spectroscopy.