The value of angle-dependent magnetoresistance (MR) synergistically and simultaneously depends on the magnitudes of magnetoresistance (MR) and magnetocrystalline anisotropy energy (MAE). In a magnetic material, the concurrence of gigantic angle-dependent MR and MR signals is rather difficult due to weak spin-lattice coupling and small MAE. Here we report the considerable magnetotransport effect in layered A-type antiferromagnetic (AFM) $\mathrm{NaCr}{\mathrm{Te}}_2$ by realigning the spin configurations. Above 3 (8) T, the antiparallel spins of adjacent layers experience a spin-flip transition to a parallel alignment along the $c$ axis ($ab$ plane). Theoretical calculations reveal that the energy band gap narrows from 0.39 to 0.11 eV, accompanying a transition from semiconductor (high-$R$ state) and half semiconductor (low-$R$ state), respectively. Thus, a gigantic negative MR ratio of −90% is obtained at 10 K. More importantly, the decrement of $R$ along $H\parallel c$ is far quicker than that of $H\parallel ab$ because the MAE of the Ising-like ferromagnetic (FM) state is $1017\mu \mathrm{eV}/{\mathrm{Cr}}^{3+}$ lower than that of XY-like FM. The distinct trends result in the angle-dependent MR ratio of 732% at 10 K. These findings unravel the intrinsic origin of magnetoresistance in $\mathrm{NaCr}{\mathrm{Te}}_2$ and will stimulate us to explore the $H$-sensitive transport property in more AFM materials.

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• Anisotropic magnetoresistance
• Magnetic phase transitions
• Magnetotransport