Two-dimensional (2D) transition metal dichalcogenides (TMDs) such as MoS2 are materials for multifarious applications such as sensing, catalysis, and energy storage. Due to their peculiar charge-transport properties, it is always desired to control their morphologies from vertical nanostructures to horizontal basal-plane oriented smooth layers. In this work, we established a low-temperature ALD process for MoS2 deposition using bis(t-butylimino)bis(dimethylamino)molybdenum(vi) and H2S precursors. The ALD reaction parameters, including reaction temperature and precursor pulse times, are systematically investigated and optimized. Polycrystalline MoS2 is conformally deposited on carbon nanotubes, Si-wafers, and glass substrates. Moreover, the morphologies of the deposited MoS2 films are tuned from smooth film to vertically grown flakes, and to nano-dots, by controlling the reaction parameters/conditions. It is noticed that our MoS2 nanostructures showed morphology-dependent optical and electrocatalytic properties, allowing us to choose the required morphology for a targeted application.