In this paper, the intrinsic impact of inner structure features on the electrochemical performances of LiNi0.6Co0.2Mn0.2O2 cathodes is for the first time systematically investigated. Three different spherical Ni0.6Co0.2Mn0.2(OH)2 precursors are successfully synthesized by controlling pH values and ammonia concentrations. Interestingly, via a further lithiation process, the final cathodes can gradually inherit the structural features, showing distinct particle arrangement and genetic orientation characteristics in the inner structures. Such a hereditary property can be well reined for customizing the grain-orientation, helping the growth of the inert crystal direction, reducing cation mixing and exposing the high active (100) or (010) lattice planes for lithiation/delithiation processes via an intrinsical way. The degree of grain-orientation of the primary particles turns out to be a critical factor in determining the long-term stability and power performances. Due to the reduced cation mixing degree and favorable lithium diffusion pathways, the ordered agglomerates with the grain growth along with [003] direction exhibit superior rate capability and good cycle stability.