Chemical vapor transport deposition (CVTD) is an effective method for preparing large tungsten coatings for space thermionic reactors. In this study, a high-density, high-work-function polycrystalline tungsten coating was prepared using a WCl6 transport agent in a concentric tube-type closed transport system. The relationship between the kinetics and the microstructures of the CVTD polycrystalline tungsten coating at the substrate temperature of 1593 K-1793 K and system pressure of 15.93 Pa-106.8 Pa was studied, which provided a basis for the preparation of high-quality tungsten coatings. At a low temperature or a low pressure, the activation energy was approximately 2 kJ/mol, the deposition rate was almost independent of the temperature changes, and the control mechanism was mass transport limited. The tungsten coating had nodules on the surface with pores in the grain boundaries and grew preferentially along <111>. At a high temperature and a high pressure, the apparent activation energy was approximately 90 kJ/mol, the value of order was approximately 1, and the control mechanism in this process range was surface limited. The tungsten coating exhibited a hexagonal pyramidal structure, and the growth direction was preferred along <110>. The average work function of the tungsten coating prepared at a temperature of 1673 K and a system pressure of 106.80 Pa was as high as 5.20 eV.