Two novel fluorescent probes L1 and L2 for recognizing Al3+ 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 Al3+, 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 Al3+ with a binding constant of 2.6×1010 M‐1. Furthermore, its fluorescence intensity exhibits a good linear relationship with Al3+ 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.