The brittleness index plays a significant role in the hydraulic fracturing design and wellbore stability analysis of shale reservoirs. Various brittleness indices have been proposed to characterize the brittleness of shale rocks, but almost all of them ignored the anisotropy of the brittleness index. Therefore, uniaxial compression testing integrated with geophysical logging was used to provide insights into the anisotropy of the brittleness index for Longmaxi shale, the presented method was utilized to assess brittleness index of Longmaxi shale formation for the interval of 3155–3175 m in CW-1 well. The results indicated that the brittleness index of Longmaxi shale showed a distinct anisotropy, and it achieved the minimum value at β = 45°-60°. As the bedding angle increased, the observed brittleness index (BI2_β) decreased firstly and increased then, it achieved the lowest value at β = 40°–60°, and it is consistent with the uniaxial compression testing results. Compared to the isotropic brittleness index (β = 0°), the deviation of the anisotropic brittleness index ranged from 10% to 66.7%, in other words, the anisotropy of brittleness index cannot be ignored for Longmaxi shale. Organic matter content is one of the main intrinsic causes of shale anisotropy, and the anisotropy degree of the brittleness index generally increases with the increase in organic matter content. The present work is valuable for the assessment of anisotropic brittleness for hydraulic fracturing design and wellbore stability analysis.