We report the structural and electrochemical characteristics of Li4/3Me5/3O4 (MeTi, Mn) spinel materials exhibiting nanostructured morphology. We have applied Raman and FTIR spectroscopy to study the local structure. Vibrational features are in good concordance with the factor group analysis (Oh 7 symmetry). The zero-strain insertion material Li4/3Ti5/3O4 delivers 150mAh/g while Li4/3Mn5/3O4 inserts 2.8 Li/mole of oxide leading to a specific capacity of 158mAh/g.