LAUSR

Boron nitride (BN) is a two‐dimensional ceramic material that has been widely applied in various catalysis reactions. However, endowing the BN material with adequate reactive centers remains to be a considerable challenge. Herein, we propose a tunable boron and nitride dual vacancies strategy to generate highly active oxygen‐doping BN (BNO) material via heat treatment in vacuum. Experimental results indicate that the vacuum treatment fabricates boron and nitride dual vacancies on the BNO. The as‐prepared vacuum treated BNO (V‐BNO) was applied as the initiator to accelerate the aerobic oxidative desulfurization (ODS) of fuel. The boosted aerobic ODS system achieves 100 % sulfur removal in 6 h, and it can be recycled 6 times without any significant performance loss. Meanwhile, the density functional theory (DFT) reveals the reaction pathway on the V‐BNO, ensuring the contribution of boron and nitride dual vacancies to the initiation of the reaction. This work highlights the vital role of dual vacancies as initiating sites for the enhanced aerobic ODS.