The finite element model of a dual-rotor system was established by Timoshenko beam element. The dual-rotor system is a coaxial rotor whose supporting structure is similar to that of an aero-engine rotor system. The inner rotor is supported by three bearings, which makes it a redundantly supported rotor. The outer rotor connects the inner rotor by an intershaft bearing. The spectrum characteristics of the dual-rotor system under unbalanced excitation and misalignment excitation were analysed in order to study the influence of coupling misalignment of the inner rotor on the spectral characteristics of the rotor system. The results indicate that the vibration caused by the misaligned coupling of the inner rotor will be transmitted to the outer rotor through the intershaft bearing. Multiple harmonic frequency components, mainly 1x and 2x, will be excited by the coupling misalignment. The amplitudes of all harmonic frequencies increase with the misalignment in both the inner and outer rotors. The vibration level of the outer rotor affected by the misalignment is lower than that of the inner rotor because it is far from the misaligned coupling. Harmonic resonance occurs when any harmonic frequencies of the misalignment response coincide with a natural frequency of the system. In order to verify the theoretical model, experiments are performed on a test rig. Both the experimental and simulation results are in good accordance with each other.