Quercetin (QCT), a flavonoid polyphenol, is the main active component responsible for the antioxidant and anti-inflammatory effects of various medicinal herbs. However, excessive intake of QCT is prone to cause adverse reactions such as vomiting and hypokalemia, so it is of great significance to establish a portable and highly sensitive method for QCT detection. Integrating fluorescence, colorimetry, and smartphone-based portable sensing into a single material matrix can achieve high-sensitivity and rapid visual multimodal synergistic detection, and significantly improve the detection accuracy and anti-interference ability through signal complementarity and mutual verification. Therefore, a single-emission blue fluorescence sensor (UNDC) based on Zr-based metal-organic framework (Zr-MOF) was prepared in this work, which exhibited a highly sensitive fluorescence quenching response to QCT with a detection limit as low as 0.59 nM. Furthermore, a dual-emission red fluorescence sensor (EuUNDC) was developed by introducing the red luminescent center Eu3+ into UNDC. EuUNDC not only maintained a sensitive fluorescence quenching response to QCT but also possessed excellent selectivity and anti-interference ability; meanwhile, it could realize colorimetric quantitative detection of QCT through UV-vis absorption spectroscopy and was successfully applied to the quantitative analysis of QCT in licorice tablets. Additionally, the portable paper sensor prepared based on EuUNDC could achieve on-site visual quantitative detection of QCT. Thus, the dual-mode fluorescent/colorimetric sensing platform constructed in this work and the smartphone-based portable sensor achieve high-sensitivity, high-selectivity, and on-site visual quantitative detection of QCT, and has broad application prospects in the field of pharmaceutical active substance analysis.