Organometallic single-precursors both aluminum and nitrogen bonded to each other have been synthesized and utilized to deposit aluminum nitride (AIN) thin films by organometallic chemical deposition (OMCVD). Compounds with the general formula $[R_2AINR'R"]_2$, ${[Me_2AIN(i-Pr)_2]_2$ ($\underline{1}$), $[Me_2AINH(i-Pr)]_2$($\underline{2}$), $[Me_2AINH(t-Bu)]_2$ ($\underline{3}$) and $[Et_2AINH(t-Bu)]_2$ ($\underline{4}$)} were synthesized and structures of $\underline{1},\underline{2},\underline{3}$ and $\underline{4}$ were characterized by Mass and NMR spectroscopy. Preparation of AIN thin films on the Si(100) single crystal surface has been examined at temperatures between 200℃ and 800℃ at $1\times10^{-4}$ Torr by OMCVD. The deposited thin films were analyzed by using Infrared, X-ray photoelectron, Xray diffraction spectroscopy and Scanning electron microscopy. The decomposition products of organometallic precursors during both OMCVD and thermolysis were analyzed by Gas chromatography (GC). The optimum temperatures for the formation of AIN thin films were found to be about 600℃ for $\underline{3}$ and about 500℃ for $\underline{4}$. The decomposition mechanism of organometallic precursors were proposed based on the decomposition studies.