Tungsten telluride WTe₂is the sole candidate of a group of two-dimensional layered transition metal dichalcogenides (TMDCs) MX₂with a thermodynamically stable 1T′-structure at room temperature. The binary system W/Te was audited with respect to a rational approach of planning and realization of a bottom-up synthesis of WTe₂nanostructures. Thus, the parameters of the synthesis via chemical vapor transports (CVT) were derived by thermodynamic simulations of the reaction pathway according to the Calphad method. Reflecting on the peritectic melting behavior at 1020 °C, the values of Δ_fHm°(298 K) = -26.5 kJ·mol^-1and Sm°(298 K) = 132 J·mol^-1·K^-1have been obtained. According to modeling, crystal growth by short time vapor transport is reasonable under the addition of bromine or TeBr₄in the temperature range between 650 and 750 °C. Experimental implementation of crystal growth of WTe₂nanosheets succeeded in a temperature gradient from 725 to 675 °C on yttria-stabilized zirconia (YSZ) (111) substrates, observing the deposition of single crystal sheets of high crystallinity with thicknesses of 15-20 nm (∼20-30 layers). The high crystallinity, pristine morphology, and overall quality of the deposited nanosheets is shown by means of atomic resolution transmission electron microscopy, selected area electron diffraction (SAED), and atomic force microscopy as well as profound double-polarized Raman spectroscopy.