Quasi-one-dimensional ZrS₃ nanoflakes attract intense interest attributed to their superior electrical and optical anisotropy, stemming from the low symmetry in the crystal structure. However, the conventional chemical vapor transport method for synthesizing bulk ZrS₃ is limited by morphology and size controllability. It is highly desirable to propose a facile way to precisely synthesize ZrS₃ nanoflakes. In this work, the chemical vapor deposition method is proposed as a feasible way to synthesize ZrS₃ nanoflakes. The effects of various substrates and temperatures on ZrS₃ synthesis have been investigated. For the as-grown ZrS₃, good crystallinity is confirmed with X-ray diffraction and transmission electron microscopy. The structure and interlayer coupling are investigated with Raman scattering spectroscopy. The strong in-plane anisotropy and interlayer coupling of the ZrS₃ nanoflakes are illustrated with angle-resolved Raman spectroscopy and temperature-dependent Raman characterization, respectively. This study demonstrates a feasible way for the synthesis of transition metal trisulfides, which may shed new light on the research of other two-dimensional anisotropic transition metal materials.