For corrosion detection, it is often desirable that a Lamb wave mode is highly sensitive to surface thinning and enjoys some degree of mode purity at a particular frequency. In view of this, this paper aims to generate a variety of Lamb wave modes over broad frequency bands to ensure an abundant supply of candidates for corrosion detection, and further, establish a strategy to find appropriate operation points efficiently and effectively. Firstly, a short-duration laser pulse is applied to generate Lamb waves over a large frequency-thickness product range. The selection of symmetric modes or anti-symmetric modes is obtained by addition or subtraction of signals captured by two identical transducers which are symmetrically coupled on both sides of the plate. Subsequently, the S0 mode at a non-dispersive frequency bandwidth is employed to improve the accuracy of the transmitter–receiver distance. Based on those, three selection criteria including mode separability, amplitude ratio and corrosion sensitivity, are presented to efficiently determine the suitable operation points (i.e., mode types and frequencies). The experimental results show that the simulated corrosion could be correctly detected and accurately localized at the chosen modes and frequencies.