The interest in tellurium nanostructures is on the rise due to their outstanding physical properties including high carrier mobility, anisotropic charge conduction, photoconductivity, thermoelectricity, and piezoelectricity. Applications in related technologies require tailoring the synthesis of tellurium from its preferred vertical growth toward the lateral growth. Here, the synthesis of pillar-like and pennette-like structures of tellurium through a powder vapor deposition technique has been discussed. It has been shown that exploiting salt additives such as NaCl in vapor deposition technique can enhance tellurium pillar dimensionality toward large planar grains. Further, we report on the synthesis of hexagonal ultrathin tellurium nanoflakes, namely tellurene, from few-layer to monolayer thickness by optimizing the growth kinetics without the usage of any additives. In addition, we explore the surface quality and physical …