The structures and dielectric properties of Pb(Fe 1=2 Nb 1=2 ) 1Àx Ti x O 3 (PFNT, x ¼ 0:07 and 0.48) single crystals were investigated using a combination of temperature-dependent dielectric, X-ray diffraction (XRD), Raman, and X-ray absorption fine structure (XAFS) spectra. Detailed structure analyses reveal that the crystal structure of PFNT (x ¼ 0:48) is single-phase tetragonal perovskite, whereas that of PFNT (x ¼ 0:07) is a mixture of rhombohedral and tetragonal phases. The structural differences are found to have significant connections with the dielectric properties in the temperature range of 90-300 K. Both samples exhibit a frequency-dependent dielectric anomaly, arising primarily from the 3d electrons hopping between Fe 2þ and Fe 3þ . The second dielectric anomaly, which is a weak frequency dispersion and observable only for PFNT (x ¼ 0:07), was probably caused by a dipole glass behavior near the morphotropic phase boundary. #