Abstract Two novel fluorescent probes L1 and L2 for recognizing Al 3+ have been prepared by cooperating salicylaldehyde‐derived Schiff base groups onto the upper rim of the calix[4]arene. Of these probes, L2 is the most effective at recognizing Al 3+ , displaying a highly selective fluorescence “on” response with an emission wavelength at 478 nm and a Stokes shift of 88 nm. Additionally, probe L2 can form a 1 : 1 coordination complex with Al 3+ with a binding constant of 2.6×10 10 M −1 . Furthermore, its fluorescence intensity exhibits a good linear relationship with Al 3+ concentration within the range of 2.0×10 −5 M to 1.4×10 −4 M, and the probe has a low detection limit of 4.36×10 −7 M.