This paper reports an investigation of the thermoelastic frictional contact responses of an elastic sphere sliding on an elastic layer-substrate system involving imperfect interfaces. The theoretical solution and numerical modeling of the thermoelastic contact of such material systems include: (1) the mathematical derivation of the closed-form frequency response functions (FRFs) of the thermoelastic field in terms of temperature, thermoelastic displacements and stresses in the layer and the substrate, (2) the numerical contact pressure determination and heat partition evaluation by employing the conjugate gradient method (CGM), and (3) stress and temperature calculations by utilizing the discrete convolution-fast Fourier transform algorithm (DC-FFT). Numerical results from the proposed model indicate that, a stronger discontinuity of interface displacements causes the contact pressure, temperature, and in-plane compressive stress to decrease, but the in-plane tensile stress, out-of-plane (compressive and tensile) stress, and von Mises stress to increase. The results also reveal the behavior transition of the out-of-plane shear stress state due to the change of the interface discontinuity status.