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Hybrid organic–inorganic composites possessing both electronic and magnetic properties are promising materials for a wide range of applications. Controlled and ordered arrangement of the organic and inorganic components is key for synergistic cooperation toward desired functions. In this work, we report the self-assemblies of core–shell composite nanofibers from conjugated block copolymers and magnetic nanoparticles through the cooperation of orthogonal non-covalent interactions. We show that well-defined core–shell conjugated polymer nanofibers can be obtained through solvent induced self-assembly and polymer crystallization, while hydroxy and pyridine functional groups located at the shell of nanofibers can immobilize magnetic nanoparticles via hydrogen bonding and coordination interactions. These precisely arranged nanostructures possess electronic properties intrinsic to the polymers and are simultaneously responsive to external magnetic fields. We applied these composite nanofibers in organic solar cells and found that these non-covalent interactions led to controlled thin film morphologies containing uniformly dispersed nanoparticles, although high loadings of these inorganic components negatively impact device performance. Our methodology is general and can be utilized to control the spatial distribution of functionalized organic/inorganic building blocks, and the magnetic responsiveness and optoelectronic activities of these nanostructures may lead to new opportunities in energy and electronic applications.