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The detection of topological phases of matter has become a central issue in recent years. Conventionally, the realization of a specific topological phase in condensed matter physics relies on probing the underlying surface band dispersion or quantum transport signature of a real material, which may be imperfect or even absent. On the other hand, quantum simulation offers an alternative approach to directly measure the topological invariant on a universal quantum computer. However, experimentally demonstrating high-dimensional topological phases remains a challenge due to the technical limitations of current experimental platforms. Here, we investigate the three-dimensional topological insulators in the AIII (chiral unitary) symmetry class, which yet lack experimental realization. Using the nuclear magnetic resonance system, we experimentally demonstrate their topological properties, where a dynamical quenching approach is adopted and the dynamical bulk-boundary correspondence in the momentum space is observed. As a result, the topological invariants are measured with high precision on the band-inversion surface, exhibiting robustness to the decoherence effect. Our Letter paves the way toward the quantum simulation of topological phases of matter in higher dimensions and more complex systems through controllable quantum phases transitions.