Objective To develop a Glypican-3 (GPC3)-targeted bimodal molecular probe for magnetic resonance imaging (MRI)/fluorescence imaging, which specifically targets liver cancer, and systematically evaluate its physicochemical properties and biological performance.Methods Bovine serum albumin (BSA)-coated gadolinium oxide (BSA@Gd2O3) nanoparticles were prepared via chemical synthesis. Indocyanine green (ICG) was loaded onto the nanoparticles through physical adsorption, and a liver cancer-targeting peptide was conjugated to the nanoparticle surface via amidation reaction. The morphological characteristics of the probe were observed using scanning electron microscopy (SEM). The hydrated particle size and Zeta potential were determined by dynamic light scattering (DLS). The ICG loading efficiency and solution stability of the probe were verified using an ultraviolet-visible (UV-Vis) spectrophotometer. The relationship between probe concentration and fluorescence intensity was measured with a fluorescence spectrophotometer, and the relaxation performance of the probe was evaluated using an MRI system. Flow cytometry was used to analyze the specific uptake of the probe by HuH-7 human hepatocellular carcinoma (HCC) cells. Additionally, the CCK-8 assay was employed to assess the effect of the probe on the proliferation of LX2 hepatic stellate cells and HuH-7 human HCC cells. Results The successfully constructed Peptide-BSA@Gd2O3-ICG probe exhibited a regular spherical morphology, with an average hydrated particle size of 133 nm (polydispersity index, PDI = 0.156) and a Zeta potential of -10.7 mV. The UV absorption spectrum of the probe showed the characteristic peak of ICG at 800 nm, and its fluorescence excitation/emission wavelengths were 777 nm and 827 nm, respectively. The probe displayed excellent MRI enhancement performance, with an R1 relaxivity of 4.57 mM-1·s-1, and the fluorescence intensity showed a linear correlation with the probe concentration. Cell uptake experiments demonstrated that the molecular probe had good targeting ability. Moreover, the probe showed almost no obvious inhibitory effect on the proliferation of LX2 cells and HuH-7 HCC cells. Conclusion The multimodal probe constructed in this study integrates specific targeting to liver cancer, excellent fluorescence imaging performance, and good biocompatibility. It is expected to provide a novel tool for the early diagnosis and precise treatment of liver cancer