An optimization procedure to find the inlet concentration profile that yields the most uniform deposition rate in a cylindrical CVD chamber has been developed. Assuming that the chemical reaction time is negligibly small, a SIMPLE based finite-volume method is adopted to solve the fully elliptic equations for momentum, temperature, and concentration. The inlet concentration profile is expressed by a linear combination of Chebyshev polynomials and the coefficients of which are determined by the local random search technique. It is shown that the present method is very effective in improving the uniformity of the deposition rate, especially when Re is high and/or the wafer is placed close to the inlet. The optimal profiles have been obtained for various Re, Gr, and geometry combinations.