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Here, we report an anisotropic giant magnetoresistance (GMR) effect and de Hass–van Alphen (dHvA) oscillation phenomena in nominal TaNiTe5 single crystals. TaNiTe5 exhibits the GMR effect with the maximum value of ∼3 × 103% at T = 1.7 K and B = 31 T, with no sign of saturation. The two-band model fitting of Hall resistivity indicates that the anomalous GMR effect was derived from the coexistence of electron and hole carriers. When the external magnetic field is applied to the electron–hole resonance, the GMR effect is enhanced. The dHvA oscillation data at multiple frequencies reveal the topological characteristics of high carrier mobility, low carrier effective mass, and a small Fermi surface pocket with a nontrivial Berry phase. Our work provides a new platform for the study of topological semimetals with significant anisotropic GMR effect.