Multimodal sensing platforms may offer reliable, fast results, but it is still challenging to incorporate biosensors with high discriminating ability in complex biological samples. Herein, we established a highly sensitive dual colorimetric/electrochemical monitoring approach for the detection of hydrogen sulfide (HS) utilizing Cu-doped In-based metal-organic frameworks (Cu/In-MOFs) combined with a versatile color selector software-based smartphone imaging device. HS can result in the enhancement of the electrochemical signal because of the electroactive substance copper sulfide (CuS), the decrease of the colorimetric signal of the characteristic absorption response caused by the strong coordination effect on Cu/In-MOFs, and the obvious changes of red-green-blue (RGB) values of images acquired via an intelligent smartphone. Attractively, the Cu/In-MOFs-based multimodal detection guarantees precise and sensitive detection of HS with triple-signal detection limits of 0.096 μM (electrochemical signals), 0.098 μM (colorimetric signals), and 0.099 μM (smartphone signals) and an outstanding linear response. This analytical toolkit provides an idea for fabricating a robust, sensitive, tolerant matrix and reliable sensing platform for rapidly monitoring HS in clinical disease diagnosis and visual supervision.