Here we argue that the angular harmonics of magnetotransport directly characterizes carrier imbalances in a multiband semimetal. A robust threefold modulation superimposed on the conventional $cos\theta$ angular Hall response is observed in ${\mathrm{WTe}}_2$ in the metallic regime at low temperatures under out-of-plane magnetic-field rotation. By tuning temperature and thickness, we demonstrate that this modulation is intrinsic and originates from enhanced nonlinear Hall response arising from its near-compensated two-band electronic structure. In contrast, a few-layer graphene exhibits a richer hierarchy of higher-order angular harmonics, consistent with its multiple dynamically distinct bands. By carefully ruling out extrinsic artefacts and employing Fourier analysis, we establish angular harmonic analysis as a sensitive probe of electronic structure in multiband semimetals.

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• Electrical properties
• Electronic structure
• Hall effect
• Magnetotransport
• Transition metal dichalcogenides
• Weyl semimetal
• Magnetoresistance