Bi is predicted to be an efficient generator of spin–orbit torques (SOTs), with charge-to-spin conversion efficiency comparable to those of prototypical heavy metals, such as Ta, W, and Pt. However, experimental reports provide widely scattered interconversion efficiencies, while the origin of the large conversion signal in Bi/Ag bilayers remains controversial. Here, we investigate charge-to-spin conversion in epitaxial and polycrystalline Bi-based magnetic heterostructures by measuring the damping-like SOT using magneto-optic Kerr effect magnetometry, complemented by structural and spectroscopic analyses and comparison with harmonic Hall resistance measurements. We show that inserting an Ag spacer between Bi(001) and metallic ferromagnets (FeCo or Ni) enhances the SOT efficiency by more than one order of magnitude, reaching an effective spin Hall conductivity of approximately $2\times {10}^5(\hslash /2e)\mathrm{S}/\mathrm{m}$, in excellent agreement with theoretical expectations for bulk Bi. This enhancement can be consistently explained by the preservation of the structural and chemical integrity of Bi—otherwise compromised by the direct deposition of a ferromagnetic overlayer—rather than by Rashba spin–orbit coupling at the Bi/Ag interface. We show that Ag forms an atomically sharp, chemically inert interface with Bi that, unlike other metallic spacers such as Al and Cu, prevents interdiffusion and solid-state dewetting while enabling efficient charge-to-spin conversion. Angle-resolved photoemission spectroscopy reveals no measurable enhancement of the Rashba spin splitting at the Bi(001) surface upon Ag deposition. Comparative studies across epitaxial, polycrystalline, and intentionally surface-oxidized Bi films, beyond oxygen doses known to destroy Bi(001) surface states, reveal that structural disorder has a negative impact on the SOT efficiency. Meanwhile, the retention of 72% of the SOT efficiency following oxygen exposure indicates a dominant bulk contribution to spin-current generation in Bi/Ag heterostructures, yielding an effective Bi spin Hall angle of approximately 1. By establishing a direct correlation between atomic-scale integrity and charge-to-spin conversion, this study provides design principles to improve the reliability of Bi-based SOT devices and offers a robust framework for interpreting spin–charge interconversion in Bi and Bi/Ag systems.

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• Crystal phenomena
• Electrical conductivity
• Electrical properties
• Electronic structure
• Growth
• Hall effect
• Kerr effect
• Magnetism
• Magnetotransport
• Roughness
• Spin-orbit coupling
• Spintronics
• Structural properties
• Surface & interfacial phenomena
• Surface states
• Transport phenomena
• Alloys
• Crystal structures
• Crystalline systems
• Device fabrication
• Devices
• Energy applications
• Ferromagnets
• Interfaces
• Magnetic multilayers
• Magnetic systems
• Magnetic thin films
• Metals
• Polycrystalline materials
• Semimetals
• Single crystal materials
• Thin films
• Two-dimensional electron system
• Annealing
• Atomic force microscopy
• Charge
• Crystallography
• Electrical transport techniques
• Electron diffraction
• Electron microscopy
• Energy-dispersive x-ray spectroscopy
• Epitaxy
• Etching
• Evaporation
• Film deposition
• Hall bar
• Magnetization measurements
• Molecular beam epitaxy
• Noncontact atomic force microscopy
• Resistivity measurements
• Sample preparation
• Scanning electron microscopy
• Transport techniques
• X-ray diffraction
• X-ray reflectivity
• X-ray techniques