Semiconductor nanowires (NWs) continue to garner significant interest in various applications ranging from nextgeneration electronics to nanoscale probes for biological systems . With cross-sectional dimensions tailorable to a few nanometers, these systems allow quantum confinement effects to emerge as electrons become quantized into discrete energy levels . In particular, core-shell nanowires give rise to additional quantum effects since mobile two-dimensional electron gases (2DEGs) can form at the semiconductor-semiconductor heterojunction interface . To fully harness the electronic properties of these systems, a wide range of material properties (such as doping density, bandgap alignment, geometry, and structural composition) may be altered to achieve spontaneous electron gas formation . While the resulting parameter space is immense, theory and predictive modeling provide a guided path for determining which combination of material properties/parameters best optimizes performance of these novel nanosystems.