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Calcium carbonate has slowly paved its way into the field of nanomaterial research due to its inherent properties: biocompatibility, pH-sensitivity, and slow biodegradability. In our efforts to synthesize calcium carbonate nanoparticles (CSCaCO₃NP) from blood cockle shells (<i>Anadara granosa</i>), we developed a simple method to synthesize CSCaCO₃NP, and loaded them with gefitinib (GEF) and paclitaxel (PTXL) to produce mono drug-loaded GEF-CSCaCO₃NP, PTXL-CSCaCO₃NP, and dual drug-loaded GEF-PTXL-CSCaCO₃NP without usage of toxic chemicals. Fourier-transform infrared spectroscopy (FTIR) results reveal that the drugs are bound to CSCaCO₃NP. Scanning electron microscopy studies reveal that the CSCaCO₃NP, GEF-CSCaCO₃NP, PTXL-CSCaCO₃NP, and GEF-PTXL-CSCaCO₃NP are almost spherical nanoparticles, with a diameter of 63.9 ± 22.3, 83.9 ± 28.2, 78.2 ± 26.4, and 87.2 ± 26.7 (nm), respectively. Dynamic light scattering (DLS) and N₂ adsorption-desorption experiments revealed that the synthesized nanoparticles are negatively charged and mesoporous, with surface areas ranging from ~8 to 10 (m²/g). Powder X-ray diffraction (PXRD) confirms that the synthesized nanoparticles are aragonite. The CSCaCO₃NP show excellent alkalinization property in plasma simulating conditions and greater solubility in a moderately acidic pH medium. The release of drugs from the nanoparticles showed zero order kinetics with a slow and sustained release. Therefore, the physico-chemical characteristics and in vitro findings suggest that the drug loaded CSCaCO₃NP represent a promising drug delivery system to deliver GEF and PTXL against breast cancer.