Surgery and subsequent chemotherapy are still the most adopted clinical modalities for bladder cancer treatments with the inevitable operation risks, chemotherapy toxicity, and high recurrence rate. Here, we report an unprecedented tumor cell dissociation strategy for malignant bladder tumor removal without the needs of conventional surgery and chemotherapy. A common metal ion chelator, ethylene diamine tetraacetic acid (EDTA), has been loaded into the interlayers of neurotensin (NT)-modified Zn-Al layered double hydroxide (LDH). Under the targeting by NT, such a nano-platform shows high affinity to bladder tumor cells, leading to the highly selective and efficient accumulation at the bladder tumor site. The released EDTA molecules deprive Ca2+ from the intercellular calcium-dependent connexin by EDTA-Ca2+ chelation, resulting in the tumor disaggregation that is then safely excreted out of body rather than killed using toxic chemodrugs, thus, ensuring excellent biosafety and extraordinarily high effectiveness.