Spin‐charge interconversion phenomena at the interface between magnetic materials and topological insulators (TIs) are attracting enormous interest in the research effort toward the development of fast and ultra‐low power devices for future information and communication technology. A large spin‐to‐charge (S2C) conversion efficiency in Au/Co/Au/Sb2Te3/Si(111) heterostructures based on Sb2Te3 TIs grown by metal–organic chemical vapor deposition on 4″ Si(111) substrates is reported. By conducting room temperature spin pumping ferromagnetic resonance, a 250% enhanced charge current due to spin pumping in the Sb2Te3‐containing system is measured when compared to the reference Au/Co/Au/Si(111). The corresponding inverse Edelstein effect length λIEE ranges from 0.28 to 0.61 nm, depending on the adopted methodological analysis, with the upper value being so far the largest observed for the …