The catalytic exchange of hydrogen isotopes is a promising technology for purifying recycled water in nuclear power stations. However, it remains a challenge for achieving high catalytic efficiency and stability at low temperatures. In this work, we propose a facile strategy to enhance the catalyst efficiency by introducing LiF in the Pt/Ti3AlC2 (Pt‐5‐LiF/Ti3AlC2). The incorporation of LiF significantly achieves high catalytic exchange efficiency of 92% and a turnover frequency of 28.1 h‐1, which are more than twice that of Pt/Ti3AlC2. The structure‐activity relationship analysis reveals that the introduction of LiF substantially enhanced the hydrogen adsorption capacity of the catalyst and further improved the performance of the catalysts. Moreover, this LiF‐added strategy is also applicable to other Pt‐based catalysts such as Pt/Al2O3 and Pt/activated carbon. This work provides a novel catalyst design strategy for high‐efficiency catalytic exchange of hydrogen isotopes.