A multi-frequency excitation method is proposed for higher efficiency of the continuous scanning laser Doppler vibration (CSLDV) measurement. First, based on the principle of a single frequency excitation for the CSLDV test, the approach of CSLDV measurement under a multi-frequency excitation is explored and the structural operational deflection shape(ODS) extraction based on a multi-frequency excitation is developed. Then, the simulation test of a beam structure is used to verify the effectiveness of the method. Finally, the experiments based on CSLDV and SLDV are both conducted on a cantilever beam structure. The results show that the structural ODS can be obtained accurately by both tests with the fact that the CSLDV method is more efficient and has higher spatial resolution than that of the SLDV method. This approach shows practical value for further engineering applications.