disturbances and produce very little stray fields, thus allowing for high-density memory integration. [1][2][3] Among them, noncollinear antiferromagnet with nontrivial spin structure has led to unconventional electromagnetic response. [4][5][6][7] When electrical current flows through a non collinear spin texture, the adjacent three spins (S i , S j , and S k ) produce nonzero scalar spin chirality S i • (S j × S k ), can induce nonzero Berry curvature in real space, which acts like a fictitious magnetic field for the conduction electrons and gives rise to the topological Hall effect (THE). [8][9][10][11][12][13][14] There are series of compounds formed between transition or rare earth metals (T) and different main group elements (M) with chemical formula T 5 M 3 . Among them, T 5 Si 3 phases crystallize with the hexagonal Mn 5 Si 3 -type structure (space group P6 3 /mcm) have been found to have complex antiferromagnetic ordering that deserve attention. [15][16][17] In Mn 5 Si 3 -type structure, there are two inequivalent Wyckoff positions of atoms T: 4(d) and 6(g) (T1 and T2, respectively), yielding two structural motifs in the unit cell [18,19] (Figure S1, 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 Cr 5 Si 3 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 Cr 5 Si 3 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 Cr 5 Si 3 nanosheet. The Cr 5 Si 3 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.