The spin Hall and orbital Hall effects are fundamental mechanisms for generating transverse spin and orbital currents. However, their intrinsic entanglement via spin-orbit coupling (SOC) has made the generation of pure spin or orbital Hall current a long-standing challenge. Here, we demonstrate a strategy not only to generate but also to reversibly switch between spin and orbital Hall currents within a single material. Combining first-principles calculations with tight-binding modeling, we show that spin-orbital-valley locking, together with external-field-controlled topological band inversion, enables a reversible crossover of Hall transport between spin- and orbital-dominated regimes, even yielding a dominant spin Hall response in weak-SOC systems. Our Letter provides a direct route toward disentangling mixed spin-orbital transport and establishes a versatile platform for the independent control and probing of spin and orbital degrees of freedom.

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• Spin Hall effect
• Spin-orbit coupling
• Valley degrees of freedom
• 2-dimensional systems
• First-principles calculations
• Tight-binding model