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There is a clinically unmet need for effective treatments for triple-negative breast cancer (TNBC), as it remains the most aggressive subtype of breast cancer. Herein, we demonstrate a promising strategy using a tumor-targeting alkylphosphocholine (NM600) for targeted radionuclide therapy of TNBC. NM600 was radiolabeled with ⁸⁶Y for PET imaging and ¹⁷⁷Lu for targeted radionuclide therapy. ⁸⁶Y-NM600 PET imaging was performed on female BALB/C mice bearing syngeneic 4T07 (nonmetastatic) and 4T1 (metastatic) TNBC tumor grafts (n = 3–5). Quantitative data derived from a PET-image region-of-interest analysis, which was corroborated by ex vivo biodistribution, were used to estimate the dosimetry of ¹⁷⁷Lu-NM600 treatments. Weight measurement, complete blood counts, and histopathology analysis were performed to determine ¹⁷⁷Lu-NM600 toxicity in naïve BALB/C mice administered 9.25 or …