A fiber-optic interferometric probe based on a two-mode fiber (TMF) is proposed and demonstrated for measuring the thermo-optic coefficients (TOCs) of liquid samples. The proposed probe can be simply fabricated by fusion-splicing a short piece of TMF to a lead single mode fiber (SMF) with small lateral offset, which makes interference between LP(01) and LP(02) modes. The sensing responses of the probe to temperature and surrounding refractive index (SRI) have been experimentally investigated to show the capability of simultaneous measurements; the phase change of the reflection spectrum was related to temperature variation and the intensity change was to SRI variation. The data analysis is made not only in the spectral domain but in the Fourier domain also to effectively quantify the measurements. The TOCs of several liquid samples including water, ethanol, and acetone have been obtained with the proposed method.