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Fluorescent quantum dots (QDs) of carbon and semiconductors have superior optical properties and show great potential in sensing applications. This paper reports a novel method for rapid detection of uranyl ions via ratiometric fluorescence signals by employing two types of QDs as the key materials. As the most soluble and stable toxic uranium species, uranyl has been recognized as an important index for nuclear industrial wastewater. However, its on-site, rapid, and sensitive determination remains challenging. This work uses the ratiometric fluorescent signal of QDs and combines a smartphone-based handheld device for on-site and rapid detection of uranyl. The ratiometric fluorescent probe is achieved by integrating carbon dots (C-dots) and CdTe QDs (MPA@CdTe QDs) through chemical hybridization. The presence of uranyl ions greatly quenches the red fluorescence of the CdTe QDs, whereas the green fluorescence keeps constant, leading to an obvious color change. An app and a 3D-printed accessory have been developed on a smartphone to analyze and calculate the content of uranyl on the basis of captured fluorescence signals from a test strip with an immobilized probe. This new designed mobile detection system displays good analytical performance for uranyl ions in a wide concentration range of 1 to 150 μM, which shows a great potential application in controlling the nuclear industrial pollution.