Traditional tone burst excitation cannot attain a high output resolution, due to the time duration. The received signal is much longer than that of excitation during the propagation, which can increase the difficulty of signal processing, and reduce the resolution. Therefore, it is of significant interest to develop a general methodology for crack quantification through the optimal design of the excitation waveform and signal-processing methods. This paper presents a new crack size quantification method based on high-resolution Lamb waves. The linear chirp (L-Chirp) signal and Golay complementary code (GCC) signal are used as Lamb wave excitation signals. After dispersion removal, these excitation waveforms, based on pulse compression, can effectively improve the inspection resolution in plate-like structures. A series of simulations of both healthy plates and plates with different crack sizes are performed by Abaqus CAE, using different excitation waveforms. The first wave package of the S0 mode after pulse compression is chosen to extract the damage features. A multivariate regression model is proposed to correlate the damage features to the crack size. The effectiveness of the proposed crack size quantification method is verified by a comparison with tone burst excitation, and the accuracy of the crack size quantification method is verified by validation experiments.