Despite the widespread industrial use of chromium-based compounds, there are concerns regarding their toxicity in biomedical applications. Herein, bimetallic calcium chromatite nanocomposite (CC) was prepared through green synthesis using Stevia rebaudiana leaf extract. A porous nanorod of CC was obtained through calcinations at 800oC. The formation of CC was confirmed by SEM (scanning electron microscopy), EDAX (Energy-dispersive X-ray spectroscopy), HRTEM (High-resolution transmission electron microscopy), TGA (Thermal gravimetric analysis), and BET (Brunauer-Emmett-Teller). The cytotoxicity of the CC was evaluated by the MTT method against cancer lines (HeLa, U87, A549) and primary cell line (HUVEC). The IC50 value of CC against cancer cell lines was lower than the primary cell lines. The calculated specificity index was greater than one, indicating that this CC might target cancer cells without the use of a targeting moiety. Gene expression studies revealed that CC upregulated the proapoptotic gene, BAX and downregulated the anti-apoptotic gene, Bcl-2, to induce apoptosis. The KDR and VEGF genes responsible for angiogenesis were down-regulated, indicating that CC decreases angiogenesis to promote apoptosis. The findings suggest CC prepared using phytoextract could be considered an adjuvant cancer therapy treatment.