Electrochemical CO₂ reduction reaction (CO₂RR) to produce value‐added multi‐carbon chemicals has been an appealing approach to achieving environmentally friendly carbon neutrality in recent years. Despite extensive research focusing on the use of CO₂ to produce high‐value chemicals like high‐energy‐density hydrocarbons, there have been few reports on the production of propane (C₃H₈), which requires carbon chain elongation and protonation. A rationally designed 0D/2D hybrid Cu₂O anchored‐Ti₃C₂T_x MXene catalyst (Cu₂O/MXene) is demonstrated with efficient CO₂RR activity in an aqueous electrolyte to produce C₃H₈. As a result, a significantly high Faradaic efficiency (FE) of 3.3% is achieved for the synthesis of C₃H₈ via the CO₂RR with Cu₂O/MXene, which is ≈26 times higher than that of Cu/MXene prepared by the same hydrothermal process without NH₄OH solution. Based on in‐situ attenuated total reflection‐Fourier transform infrared spectroscopy (ATR‐FTIR) and density functional theory (DFT) calculations, it is proposed that the significant electrocatalytic conversion originated from the synergistic behavior of the Cu₂O nanoparticles, which bound the *C₂ intermediates, and the MXene that bound the *CO coupling to the C₃ intermediate. The results disclose that the rationally designed MXene‐based hybrid catalyst facilitates multi‐carbon coupling as well as protonation, thereby manipulating the CO₂RR pathway.

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