Higher levels of fluoride (F-) in groundwater constitute a severe problem that affects more than 200 million people spread over 25 countries. It is essential not only to detect but also to accurately quantify aqueous F- to ensure safety. The need of the hour is to develop smart water quality testing systems that would be effective in location-based real-time water quality data collection, devoid of professional expertise for handling. We report a cheap, handheld, portable mobile device for colorimetric detection and rapid estimation of F- in water by the application of the synthesized core-shell nanoparticles (near-cubic ceria@zirconia nanocages) and a chemoresponsive dye (xylenol orange). The nanomaterial has been characterized thoroughly, and the mechanism of sensing has been studied in detail. The sensor system is highly selective toward F- and shows unprecedented sensitivity in the range of 0.1-5 ppm of F-, in field water samples, which is the transition regime, where remedial measures may be needed. It addresses multiple issues expressed by indicator-based metal complexes used to determine F- previously. Consistency in the performance of the sensing material has been tested with synthetic F- standards, water samples from F- affected regions, and dental care products like toothpastes and mouthwash using a smartphone attachment and by the naked eye. The sensor performs better than what was reported by prior works on aqueous F- sensing. © 2020 American Chemical Society.