Despite enormous expenditures in the research field, the electron-doped side of nickelate superconductors remains uncharted territory. Substituting the trivalent rare-earth cations by a tetravalent one hitherto failed. Here, we demonstrate by first-principles calculations a disorder-free route to electron dope Ruddlesden-Popper nickelates. When intercalating wide-band-gap insulating layers such as LaO (=Al, Ga, Sc) into LaNiO, the extra (LaO) layers act as electron donors, releasing carriers into the Ni-3 orbitals. This electron doping puts LaNiO:LaAlO naturally in the optimal region for -wave superconductivity with T exceeding 50 K. The same concept also allows us to electron dope LaNiO, the superconductor in the limelight.

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