A naphthol and nitro‐aniline‐based fluorometric and colorimetric chemosensor BHMN, 1,1‐bis(2‐(((E)‐(2‐hydroxy naphthalene‐1‐yl)methylene)amino)ethyl)‐3‐(4‐nitrophenyl)thiourea, was synthesized. Sensor BHMN detected Al3+ with fluorescence turn‐on and Fe3+ via color variation of colorless to purple. Binding ratios of BHMN to Al3+ and Fe3+ turned out to be 1 : 1. Detection limits for Al3+ and Fe3+ by BHMN were analyzed to be 8.22 μM and 3.10 μM. Additionally, the naked‐eye test strip was applied for sensing Fe3+ and showed that BHMN could effectively discriminate Fe3+ from Fe2+ and other cations. The binding mechanisms of BHMN to Al3+ and Fe3+ were identified by ESI‐mass, Job plot, NMR titration, and DFT calculations.