Tuning the dielectric properties via composition-tailoring is demonstrated for variable-lithium, constant titanium co-doped nickel oxide (LixTi0.1Ni1-xO; x = 0.05-0.30; referred to LTNO). The effect of variable Li-content on the structure and dielectric properties of LTNO is investigated. X-ray diffraction studies confirm the formation of a cubic NiO phase in LTNO for x=0.05-0.30. However, lattice parameter reduction was evident with increasing Li-content. Composition-driven giant dielectric constant (10(4)-10(5)) was observed for a higher lithium content (x = 0.15-0.30) leading to realization of LTNO ceramics. The origin of the high dielectric constant observed in these low density LTNO ceramics is attributed to the Maxwell-Wagner polarization mechanism. (C) 2016 Elsevier B.V. All rights reserved.