Anions play an indispensable role in the balance and regulation of the ecological environment and human health; however, excess anions can cause serious ecological and environment problems. Therefore, the detection and removal of excess anions in aqueous solution is not only a technological problem but also crucial for environmental protection. Herein, a set of water-soluble pyrene-based cationic fluorophores were synthesized, which exhibit high sensitivity for the detection of the anions BF4–, PF6–, and ClO4– via electrostatic interactions. Such fluorescent probes exhibit "turn-on" emission characteristics even at low concentrations of anions due to anion-π+ interactions. Moreover, these fluorescence probes act as efficient precipitating agents for the removal of the BF4–, PF6–, and ClO4– anions from an aqueous environment. This work opens up new avenues for future research on pyrene-based fluorophores as turn-on fluorescence probes for anion detection and as excellent precipitating agents in environmental settings.