Comprehensive SummaryThe strong oxophilicity of actinide complexes prevents their applications in the transformation of oxygen‐containing substrates. Herein, we report the use of a uranium(IV) alkyl complex as a catalyst for the hydroboration of carbonyl compounds. This reaction has good functional group tolerance and chemo‐selectivity under mild conditions. This study represents the rare example of catalytic reaction promoted by a uranium alkyl complex and highlights the potential of uranium complexes in synthetic chemistry.