Two-dimensional (2D) layered materials have stimulated extensive research interest for their unique thickness-dependent electronic and optical properties. However, the layer-number-dependent studies on 2D materials date are largely limited to exfoliated flakes with relatively small lateral size and poor yield. The direct synthesis of 2D materials with a precise control of the number of atomic layers remains a substantial synthetic challenge. Here we report a systematic study of chemical vapor deposition synthesis of large-area atomically thin 2D nickel telluride (NiTe2) single crystals and investigate the thickness dependent electronic properties. By controlling the growth temperature, we show that the highly uniform NiTe2 single crystals can be synthesized with precisely tunable thickness varying from 1, 2, 3,... to multilayers with a standard deviation (similar to 0.3 nm) of less than the thickness of a monolayer layer NiTe2. Our studies further reveal a systematic evolution of single crystal domain size and nucleation density with the largest lateral domain size up to similar to 440 mu m. X-ray diffraction, transmission electron microscopy, and high resolution scanning transmission electron microscope studies demonstrate that the resulting 2D crystals are high quality single crystals and adopt hexagonal 1T phase. Electrical transport studies reveal that the 2D NiTe2 single crystals show a strong thickness-tunable electrical properties, with an excellent conductivity up to 7.8 X 10(5) S m(-1) and extraordinary breakdown current density up to 4.7 X 10(7) A/cm(2). The systematic study and robust synthesis of NiTe2 nanosheets defines a reliable chemical route to 2D single crystals with precisely tailored thickness and could enable the design of new device architectures based on thickness-tunable electrical properties.