The selective excitation of coherent anti-Stokes Raman scattering(CARS)to the νs(CH₃)(2832 cm^-1)and the νAS(CH₃)(2948 cm^-1 )vibrational modes from methanol solution is successfully achieved by adaptive femtosecond pulse shaping coherent control technology. In order to explore the mechanism of mode-selective excitation from two-pulse femtosecond CARS spectrum,second harmonic generation frequency-resolved optical gating(SHG-FROG)method is used to measure the original and optimal pump pulses. SHG-FROG traces indicate that the mode-selective excitation of femtosecond CARS spectrum can be achieved by manipulating the effective frequency components of the pump pulse related to specific molecular vibrational mode. The experimental results demonstrate that adaptive femtosecond pulse shaping coherent control technology has scientific significance for the complicated molecular systems.