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The antimony selenide (Sb2Se3) thin film solar cells technology become promising due to its excellent anisotropic charge transport and brilliant light absorption capability. Especially, the device performance heavily relies on the vertically oriented Sb2Se3 grain to promote photoexcited carrier transport. However, crystalline orientation control has been a major issue in Sb2Se3 thin film solar cells. In this work, a new strategy has been developed to tailor the crystal growth of Sb2Se3 ribbons perpendicular to the substrate by using the structural heterostructured CdS buffer layer. The heterostructured CdS buffer layer was formed by a dual layer of CdS nanorods and nanoparticles. The hexagonal CdS nanorods passivated by a thin cubic CdS nanoparticle layer can promote [211] and [221] directional growth of Sb2Se3 ribbons using a close space sublimation approach. The improved buffer/absorber interface, reduced interface defects, and recombination loss contribute to the improved device efficiency of 7.16%. This new structural heterostructured CdS buffer layer can regulate Sb2Se3 nanoribbons crystal growth and pave the way to further improve the low-dimensional chalcogenide thin film solar cell efficiency.