Fibers are among the most versatile material forms in contemporary applications, including textiles, biomedicine, and aerospace. Wet spinning, the process of coagulating a polymer solution into tangible fibers, remains one of the oldest and most reliable methods for continuously fabricating fibers from a wide range of materials. Contemporary research in fiber science has begun to re-imagine filaments as environmentally-responsive materials, capitalizing on novel classes of polymers and nanomaterials to amplify sensing, electrical, and mechanical properties. A promising class is aromatic organic materials, which can offer distinctive processability and structural advantages with tunable intermolecular interactions such as aromatic stacking and hydrogen bonding. In this thesis, we focus on the controlled assembly and processing of anisotropic building blocks, from thermotropic LC monomers to aramid nanofibers, for the preparation of responsive filaments. In understanding their interactions and ordering, we formulate and design wet spinning processes to scalably fabricate thermoresponsive filaments for applications in active textiles, artificial muscles, and atmospheric water harvesting.