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Abstract MXenes constitute a rapidly growing family of 2D materials that are promising for optoelectronic applications because of numerous attractive properties, including high electrical conductivity. However, the most widely used titanium carbide (Ti₃C₂T_x) MXene transparent conductive electrode exhibits insufficient environmental stability and work function (WF), which impede practical applications Ti₃C₂T_xelectrodes in solution‐processed optoelectronics. Herein, Ti₃C₂T_xMXene film with a compact structure and a perfluorosulfonic acid (PFSA) barrier layer is presented as a promising electrode for organic light‐emitting diodes (OLEDs). The electrode shows excellent environmental stability, highWFof 5.84 eV, and low sheet resistanceR_Sof 97.4 Ω sq⁻¹. The compact Ti₃C₂T_xstructure after thermal annealing resists intercalation of moisture and environmental contaminants. In addition, the PFSA surface modification passivates interflake defects and modulates theWF. Thus, changes in theWFandR_Sare negligible even after 22 days of exposure to ambient air. The Ti₃C₂T_xMXene is applied for large‐area, 10 × 10 passive matrix flexible OLEDs on substrates measuring 6 × 6 cm. This work provides a simple but efficient strategy to overcome both the limited environmental stability and lowWFof MXene electrodes for solution‐processable optoelectronics.