The past decades have witnessed an increasing interest in the exploration of room temperature gallium-based liquid metal (LM) in the field of microfluidics, soft robotics, electrobiology, and biomedicine. Herein, this study for the first time reports the utilization of nanosized gallium-indium eutectic alloys (EGaIn) as a radiosensitizer for enhancing tumor radiotherapy. The sodium alginate (Alg) functionalized EGaIn nanoparticles (denoted as EGaIn@Alg NPs) are prepared via a simple one-step synthesis method. The coating of Alg not only prevents the aggregation and oxidation of EGaIn NPs in an aqueous solution but also enables them low cytotoxicity, good biocompatibility, and in-situ formation of gels in the Ca2+ enriched tumor physiological microenvironment. Due to the metallic nature and high density, EGaIn can increase the generation of reactive oxygen species under the irradiation of X-ray, which can not only directly promote DNA damage and cell apoptosis, but also show an efficient tumor inhibition rate in vivo. Moreover, EGaIn@Alg NPs hold good performance as computed tomography (CT) and photoacoustic tomography (PAT) imaging contrast agents. This work provides an alternative nanotechnology strategy for tumor radiosensitization and also enlarges the biomedical application of gallium-based LM.