We show that the NiO6 crystal field energies can be tailored indirectly via heterovalent A cation ordering in layered (La,A) NiO4 Ruddlesden-Popper (RP) oxides, where A = Sr, Ca, or Ba, using density functional calculations. We leverage as a driving force the electrostatic interactions between charged [LaO](1+) and neutral [AO](0) planes to inductively tune the Ni-O bond distortions, without intentional doping or epitaxial strain, altering the correlated d-orbital energies. We use this strategy to design cation ordered LaCaNiO4 and LaBaNiO4 with distortions favoring enhanced Ni e(g) orbital polarization, and find local electronic structure signatures analogous to those in RP La-cuprates, i.e., parent phases of the high-temperature superconducting oxides. (C) 2014 Author(s).