Chemotherapy is one of the major cancer therapeutic approaches, however, it is limited by non-specificity, poor solubility, resistance. We reported here the use of bioresponsive nano metal azolate framework-4 (MAF-4) as vehicle materials and cRGD (cyclic arginine-glycine-aspartic) as target peptide to precisely deliver PSeD (selenadiazole derivative) to breast cancer cells. This intelligent nanosystem was stable at relatively basic pH (similar to 7.4, body fluid), while it slowly decomposed at slightly acidic pH (similar to 5.3, lysosomes) to release drug for precise treatment of breast cancer. The nanosystem specifically accumulated in tumors in vivo, and thus demonstrated high antitumor efficacy and non-toxic to normal tissues. Generally, this study indulged an innovative strategy for efficient cancer therapy using intelligent nanocarrier materials.