The relaxation processes correlated to atomic defects were investigated by the internal friction method using a multifunctional internal friction apparatus for TiMo alloys. The microstructures of the TiMo alloys with different Mo content and heat treatments were observed using an optic microscopy and a scanning electronic microscopy. Their phase constitutions were detected by X-ray diffraction (XRD). The ¢ phase increases and ¡ phase decreases in volume with increasing Mo content for the furnace-cooled alloys. Similarly, the ¢ M phase volume increases when Mo content is increased. The two relaxational internal friction peaks, named as P1 for the low temperature peak and P2 for the high temperature peak, respectively, are found on the internal friction temperature dependent curves in the alloys. The two peaks always appear in the present experimental specimens with different Mo content and different heat treatments except for the water quenched Ti24 Mo alloys. The P1 and P2 peaks are all influenced by Mo content and heat treatments and related to phase constitutions and microstructures. The P1 peak height increases with increasing Mo content for the water quenched alloys and the P1 peak temperature is not changed with Mo content. The P2 peak height increases also with increasing Mo content and the P2 peak temperature is raised when Mo content is increased but for the water quenched Ti3Mo and Ti5Mo alloys. Relaxation parameters of P1 peak are H wq1 = 1.56 « 0.1 eV and¸0 wq1 = 2.5 © 10 ¹16«0.1 s and those of P2 peak are H wq2 = 2.3 « 0.1 eV and¸0 wq2 = 2.1 © 10 ¹17«0.1 s for the water-quenched Ti5Mo alloy, respectively. The P1 peak is attributed to the stressinduced short-range ordering of oxygen complexes around Ti atoms in the TiMo alloys. The increase of the P1 peak height with increasing Mo content is attributed to the increase of ¢ phase in volume. The P2 peak is resulted from the interaction of MoO atoms or the reorientation of MoMo atomic pairs by means of vacancies. The MoO interaction is strengthened when Mo content is increased, which results in the increase of both the peak temperature and the activation energy of the P2 peak.