An inorganic-organic hybrid probe MP-ZIF-90 was synthesized via a simple condensation reaction based on the free CHO groups of zeolitic imidazolate framework-90 (ZIF-90) and 4-methyl-1-(4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl)pyridinium bromide (MP). This probe exhibited intense green emission, which was selectively quenched by the addition of ClO- anions. The response of probe MP-ZIF-90 toward ClO- was rapid (within 20 s) and sensitive, with a limit of detection (LOD) of 0.612 μM. Importantly, the utilization of the probe in the fluorescence imaging of ClO- anions in the mitochondria of living cells and zebrafish was demonstrated.