Anisotropic materials formed by living organisms possess remarkable mechanical properties due to their intricate microstructure and directional freedom. In contrast, human‐made materials face challenges in achieving similar levels of directionality due to material and manufacturability constraints. To overcome these limitations, an approach using 3D printing of self‐assembling thermotropic liquid crystal polymers (LCPs) is presented. Their high stiffness and strength is granted by nematic domains aligning during the extrusion process. Here, a remarkably wide range of Young's modulus from 3 to 40 GPa is obtained by utilizing directionality of the nematic flow the printing process. By determining a relationship between stiffness, nozzle diameter, and line width, a design space where shaping and mechanical performance can be combined is identified. The ability to print LCPs with on‐the‐fly width changes to accommodate arbitrary spatially varying directions is demonstrated. This unlocks the possibility to manufacture exquisite patterns inspired by fluid dynamics with steep curvature variations. Utilizing the synergy between this path‐planning method and LCPs, functional objects with stiffness and curvature gradients can be 3D‐printed, offering potential applications in lightweight sustainable structures embedding crack‐mitigation strategies. This method also opens avenues for studying and replicating intricate patterns observed in nature, such as wood or turbulent flow using 3D printing.