MXene sheets, as new 2D nanomaterials, have been used in many advanced applications due to their superior thin-layered architecture, as well as their capability to be employed as novel nanocontainers for advanced applications. In this research, intercalated Ti3C2 MXene sheets were synthesized through an etching method, and then they were modified with 3-aminopropyltriethoxysilane (APTES). Cerium cations (Ce3+) as an eco-friendly corrosion inhibitor were encapsulated within Ti3C2 MXene sheets to fabricate novel self-healing epoxy nanocomposite coatings. The corrosion protection performance (CPP) of Ce3+-doped Ti3C2 MXene nanosheets (Ti3C2 MXene-Ce3+) in a 3.5 wt % sodium chloride (NaCl) solution was studied on bare mild steel substrates using electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization measurements. The self-healing CPP of epoxy coatings loaded with 1 wt % undoped and doped Ti3C2 MXene was evaluated using EIS, salt spray, and field emission scanning electron microscopy (FE-SEM) techniques. The introduction of Ti3C2 MXene-Ce3+ into the corrosive solution and artificially scribed epoxy coating enhanced the total impedance from 717 to 6596 Ω cm2 and 8876 to 32092 Ω cm2, respectively, after 24 h of immersion compared to the control samples.