Photo-Fenton process is acknowledged for its high efficiency and technical feasibility in water treatment; however, its application is constrained by the addition of iron ions and hydrogen peroxide (H2O2). Herein, an efficient photo-self-Fenton system with coating Fe-doped carbon dots (Fe-CDs) on the surface of highly crystalline C3N5 (HC-C3N5) nanosheets was developed for degradation of tetracycline (TC) under visible light irradiation. Experimental results reveal that Fe-CDs not only serve as active sites for facilitating superior light-induced charge separation and transfer towards the in-situ generation of H2O2 over HC-C3N5, but also provide the solid-phase Fe species for maximizing the activation of in-situ generated H2O2 to produce highly oxidative OH and O2– species towards the photo-self-Fenton reaction. This research presents a novel design approach of utilizing a Fe-CDs-based photo-self-Fenton system for efficient wastewater treatment.