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Abstract Spin excitations, including magnons and spinons, can carry thermal energy and spin information. Studying spin‐mediated thermal transport is crucial for spin caloritronics, enabling efficient heat dissipation in microelectronics and advanced thermoelectric applications. However, designing quantum materials with controllable spin transport is challenging. Here, highly textured spin‐chain compound Ca₂CuO₃is synthesized using a solvent‐cast cold pressing technique, aligning 2D nanostructures with spin chains perpendicular to the pressing direction. The sample exhibits high thermal conductivity anisotropy and an excellent room‐temperature thermal conductivity of 12 ± 0.7 W m⁻¹K⁻¹, surpassing all polycrystalline quantum magnets. Such a high value is attributed to the significant spin‐mediated thermal conductivity of 10 ± 1 W m⁻¹K⁻¹, the highest reported among all polycrystalline quantum materials. Analysis through a 1D kinetic model suggests that near room‐temperature, spinon thermal transport is dominated by coupling with high‐frequency phonons, while extrinsic spinon‐defect scattering is negligible. Additionally, this method is used to prepare textured La₂CuO₄, exhibiting highly anisotropic magnon thermal transport and demonstrating its broad applicability. A distinct role of defect scattering in spin‐mediated thermal transport is observed in two spin systems. These findings open new avenues for designing quantum materials with controlled spin transport for thermal management and energy conversion.