Numerical modeling results for the primary breakup of the round nonturbulent liquid jets in shear-laden gaseous crossflow at atmospheric pressure are presented in this article. A coupled level set and volume of fluid method together with the large eddy simulation turbulence model implemented in the computational fluid dynamics (CFD) open source solver library (OpenFOAM (R)) are applied to simulate the primary breakup and to track the gas-liquid interface accurately. In the volume of fluid method, the volume fraction is advected algebraically using a compression scheme. To simulate the shear-laden crossflow, linear velocity profiles with various positive and negative slopes are considered at the inlet boundary condition. Based on the average crossflow velocity, two values of Weber number, 50 and 100, and for each of them, two values of liquid-to-gas momentum flux ratio, 5 and 20, are considered. The effect of crossflow nonuniformity on the liquid jet penetration, the location of column breakup point, and the liquid surface waves are investigated and compared with the experimental and numerical results in the literature. The results indicate that nonuniform crossflow has considerable effects on the liquid jet behavior especially on its penetration height and column breakup point. While the liquid is injected from the top of the computational domain and the positive y direction is downward, a parameter is defined as the ratio of gas velocities at the bottom and top of the inlet boundary to display the slope of the linear velocity profiles. The crossflow nonuniformity effect is magnified when the mentioned parameter increases, resulting in a significant increase of the liquid jet penetration height. Moreover, general correlations for liquid penetration height, based on experimental and numerical results, are developed in this study.