Photoluminescent metal-organic frameworks (MOFs) were grown in a living plant (Syngonium podophyllum) via immersing their roots in an aqueous solution of disodium terephthalate and terbium chloride hexahydrate sequentially for 12 h without affecting their viability. Then, app-assisted living MOF-plant nanobiohybrids were used for the detection of various toxic metal ions and organic pollutants. Their performance and sensing mechanism were also evaluated. The results demonstrated that the living plants served as self-powered preconcentrators via their passive fluid transport systems and accumulated the pollutants around the embedded MOFs, resulting in relative changes in fluorescence intensity. Therefore, the living MOF-plant nanobiohybrids initiate superior selectivity and sensitivity (0.05-0.5 μM) in water for Ag+, Cd2+, and aniline with a "turn-up" fluorescence response and for Fe3+ and Cu2+ with "turn-down" fluorescence response in the linear range of 0.05-10 μM with excellent precision and accuracy of 5 and 10%, respectively. With the easy-to-read visual signals under ultraviolet light, the app translates plant luminescent signals into digital information on a smartphone for on-site monitoring of environmental pollutants with high sensitivity and specificity. These results suggest that interfacing synthetic and living materials may contribute to the development of smart sensors for on-site environmental pollutant sensing with high accuracy.