Heteroatom-doped photoluminescent (PL) carbon dots (CDs) have recently gained attention as optical sensors due to their excellent tunable properties. In this work, we propose a one-pot hydrothermal synthesis of PL nitrogen (N), sulfur (S), and phosphorus (P) co-doped carbon dots (NSP-CDs) using glutathione and phosphoric acid (HPO) as precursors. The synthesized NSP-CDs were characterized using different spectroscopic and microscopic techniques, including ultraviolet-visible (UV-Vis) spectroscopy, fluorescence spectroscopy, Fourier-transform infrared (FTIR), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) analysis. The NSP-CDs exhibited excellent PL properties with green emission at 492 nm upon excitation at 417 nm, a high quantum yield of 26.7%, and dependent emission behavior. The as-prepared NSP-CDs were spherical with a well-monodispersed average particle size of 5.2 nm. Moreover, NSP-CDs demonstrate high PL stability toward a wider pH, high salt ionic strength, and various solvents. Furthermore, the NSP-CDs showed a three-state "off-on-off" PL response upon the sequential addition of Al and Fe ions, with a low limit of detection (LOD) of 10.8 nM for Al and 50.7 nM for Fe. The NSP-CD sensor can construct an INHIBIT logic gate with Al and Fe ions as the chemical inputs and emissions as the output mode. Owing to an excellent tunable PL property and biocompatibility, the NSP-CDs were applied for sensing Al and Fe ions as well as live cell imaging. Furthermore, NSP-CDs were designed as PL sensors for detecting Al and Fe ions in real water show their potential application.