Ln(2)Ti(2)O(7) (Ln=Y and Gd) pyrochlore glass-ceramics have been fabricated successfully via internal crystallization. Subsequently, the phase evolution from Ln(2)Ti(2)O(7) pyrochlores to Ln(0.5)U(0.5)Ti(2)O(6) brannerites in glass with uranium (U) substitutions on the Ln-site of Ln(2)Ti(2)O(7) has been investigated using X-ray diffraction, scanning electron microscope-electron dispersive spectroscopy, transmission electron microscopy, Raman and diffuse reflectance spectroscopy. Combined characterization by XRD, SEM-EDS and TEM SAED confirms the structures and phase evolution while Raman spectroscopy reveals characteristic vibration modes for both pyrochlore and brannerite. In addition, DRS of the U5+ ion has been used to probe the phase evolution, with the corresponding f-f transition band of F-2(7/2) energy level significantly shifting to longer wavenumbers due to the local coordination environment changing from eightfold coordination in pyrochlore to sixfold coordination in brannerite.