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Sulfur quantum dots (SQDs), as a novel metal-free fluorescent material, are getting increasingly tremendous attention in metal ion detection, especially for Fe3+, due to the merits of antimicrobial potential, low toxicity, and exciting optoelectronic properties. However, sensing mechanism of SQD based fluorescent probe for Fe3+ is not clear yet, and high sensitivity and large detection range remain a challenge. Here, we report the synthesis of hydrophilic SQDs as a fluorescent nanoprobe for Fe3+ via a fluorescent turn-off mode. We systematically studied the quenching mechanism by ultraviolet–visible absorption spectra, steady-state and time-resolved photoluminescent spectra, and temperature-dependent quenching constants. Results unclearly evidenced the quenching behavior to both inner filter effect and static quenching. Furthermore, the nanoprobe presents a large detection range from 2.5 to 700 μM and a limit of detection low to 53.6 nM, both of which are the record performance to our knowledge. At last, it shows high selectivity toward Fe3+ and presents no ionic strength effect in the range of investigation, which enables surprising results for Fe3+ detection in deionized water with interference ion and real water samples. [Display omitted] • A novel fluorescent nanoprobe based on sulfur quantum dots for Fe3+ was reported. • The nanoprobe delivers a record detection range and limit of detection. • The sensing mechanism is systematically studied and uncovered. • The nanoprobe shows high selectivity and results for Fe3+ in real water samples. [ABSTRACT FROM AUTHOR]