In the combustion chamber of scramjets, fuel jets interact with supersonic airflow in the form of a liquid jet in crossflow (LJIC). It is difficult to achieve adequate jet–crossflow mixing and the efficient combustion of fuel in an instant. Large eddy simulation (LES), the coupled level-set and volume of fluid (CLSVOF) method, and an adaptive mesh refinement (AMR) framework are used to simulate supersonic LJICs in this article. This way, LJIC atomization characteristics and mechanisms can be further explored and analyzed in detail. It is found that the surface waves of the liquid column exist in a two-dimensional form, including vertical and spanwise directions. Column breakup occurs when all the spanwise surface waves between adjacent vertical surface waves break up. Bow shock waves, composed of multiple connected arcuate shock waves, are dynamic and will change with the evolution of the liquid column. The vortex ring movement of supersonic LJICs, whose trends in the vertical and spanwise directions are different, is relatively complex, which is due to the complex and time-dependent shape of liquid columns.