Hyperbolic materials are highly anisotropic optical media that provide valuable assistance in emission engineering, nanoscale light focusing, and scattering enhancement. Recently discovered organic hyperbolic materials (OHMs) with exceptional biocompatibility and tunability offer promising prospects as next-generation optical media for nanoscopy, enabling superresolution bioimaging capabilities. Nonetheless, an OHM is still less accessible to many researchers because of its rarity and narrow operating wavelength range. Here, we employ first-principles calculations to expand the number of known OHMs, including conjugated polymers with multiple assembly units. Through the systematic investigation of structural and optical properties of the target copolymers, we discover extraordinary multiband hyperbolic dispersions from candidate OHMs. This approach provides a new perspective on the molecular-scale design of broadband, low-loss OHMs. It aids in identifying potential hyperbolic material candidates applicable to optical engineering and super-resolution bioimaging, offering new insights into nanoscale light–matter interactions.