Lightning rods are effective to prevent lightning damage in power systems. However, under the influence of severe weather conditions, they often face failure problems, mainly manifested as tilt and fracture caused by bolt loosening which can result in significant economic losses. Therefore, it is very meaningful to detect the loosening of the lightning rod. The vibration-based method is an effective method for bolt loosening detection and is suitable for use on large lightning rods. This paper built a finite element model of the lightning rod Flange-Bolt Structure Unit (FBSU) based on the virtual material method, designed an effective acquisition test of the vibration signal under different loosening conditions of the lightning rod FBSU. The experimental results showed that it was effective to establish the dynamic model of the lightning rod FBSU by using the virtual material method. According to the measured vibration signal, the frequency response function was obtained by TIME MDOF method, and the preliminary judgment of bolt loosening can be realized. This study lays the foundation for the precise positioning and the extent of loosening detection of lightning rod bolt loosening, and also provides a guideline for the vibration test design of large bolted structures similar to lightning rods.