netic layered transition-metal oxyhalides in a low-symmetry orthorhombic structure provide a new degree of freedom to modulate magnetism, [3] increasing the attention to explore their low-dimensional properties. [4][5][6] Recently, magnetic superstructures and optical anisotropies have been explored in layered single-crystal CrOCl. [4] Additionally, the atomic structure, work function, and magnetism of VOCl have been investigated. [5] Interestingly, relatively high Néel temperatures in monolayer FeOX (X = F, Cl, Br, or I) have recently been predicted by theoretical calculations, indicating that they are robust antiferromagnets. [7] Bulk FeOCl was first synthesized by Goldsztaub in 1935 [8] and it was reported to have the highest Néel temperature of 92 K among transition-metal oxyhalides. [4,5,9,10] It has been widely studied, specifically for its structure, [8,11,12] intercalation, [13][14][15][16][17] magnetism, [6,9,12,18] phase transition, [18,19] and catalytic performance. [20][21][22][23] Over the past decade, various methods, including chemical vapor transport (CVT), [8,[11][12][13][14][15][16][17][18][19][20][21][24][25][26] chemical vapor deposition, [27] partial pyrolysis, [22,23,28] liquid exfoliation, [29] chemical exfoliation, [6] and rapid thermal annealing, have been developed to 2D van der Waals (vdW) transition-metal oxyhalides with low symmetry, novel magnetism, and good stability provide a versatile platform for conducting fundamental research and developing spintronics. Antiferromagnetic FeOCl has attracted significant interest owing to its unique semiconductor properties and relatively high Néel temperature. Herein, good-quality centimeter-scale FeOCl single crystals are controllably synthesized using the universal temperatureoscillation chemical vapor transport (TO-CVT) method. The crystal structure, bandgap, and anisotropic behavior of the 2D FeOCl are explored in detail. The absorption spectrum and electrical measurements reveal that 2D FeOCl is a semiconductor with an optical bandgap of ≈2.1 eV and a resistivity of ≈10 −1 Ω m at 295 K, and the bandgap increases with decreasing thickness. Strong in-plane optical and electrical anisotropies are observed in 2D FeOCl flakes, and the maximum resistance anisotropic ratio reaches 2.66 at 295 K. Additionally, the lattice vibration modes are studied through temperature-dependent Raman spectra and first-principles density functional calculations. A significant decrease in the Raman frequencies below the Néel temperature is observed, which results from the strong spin−phonon coupling effect in 2D FeOCl. This study provides a highquality low-symmetry vdW magnetic candidate for miniaturized spintronics.