LAUSR

Antiferromagnets with noncollinear spin order are expected to exhibit unconventional electromagnetic response, such as spin Hall effects, chiral abnormal, quantum Hall effect, and topological Hall effect. Here, 2D thickness‐controlled and high‐quality Cr5Si3 nanosheets that are compatible with the complementary metal‐oxide‐semiconductor technology are synthesized by chemical vapor deposition method. The angular dependence of electromagnetic transport properties of Cr5Si3 nanosheets is investigated using a physical property measurement system, and an obvious topological Hall effect (THE) appears at a large tilted magnetic field, which results from the noncollinear magnetic structure of the Cr5Si3 nanosheet. The Cr5Si3 nanosheets exhibit distinct thickness‐dependent perpendicular magnetic anisotropy (PMA), and the THE only emerges in the specific thickness range with moderate PMA. This work provides opportunities for exploring fundamental spin‐related physical mechanisms of noncollinear antiferromagnet in ultrathin limit.