Abstract: To explore the feasibility of laser solidification technology in the treatment of high-level radioactive waste containing molybdenum, a fiber continuous laser was performed on borosilicate glasses with varying MoO₃ contents by employing a fiber continuous laser. The samples were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and Raman spectroscopy. It was indicated by XRD and SEM analyses that the solid solubility limit of MoO₃ in this borosilicate glass system is approximately 4 wt%. Below this limit, a smooth glass phase was exhibited by the samples. When the MoO₃ content was increased to 5 wt%, CaMoO₄ crystals were precipitated from the samples. It was revealed by Raman analysis that a decrease in the polymerization degree of the borosilicate glass network structure is led to by the introduction of MoO₃, by which a depolymerizing effect is exerted on the glass structure. Additionally, the density of the solidified body was increased from 2.53 g/cm³ to 2.56 g/cm³ by the addition of MoO₃, by which the compactness of the glass was enhanced. The potential application of laser technology in the field of nuclear waste glass solidification treatment is verified by this study.