Dual-ion mobilities of Na organic batteries are investigated with in-situ XRD analysis and computational estimation considering molecular alignments in the solid state, signifying the interactive variations of ionic-pairs of an ionic liquid electrolyte and an antiaromatic molecule, nickel(II) norcorrole (NiNc). An appropriate cavity sphere in three-dimensional molecular alignments dispensed mobilities of dual-ion in an ionic liquid, resulting in high battery capacities, supplemented with the comparison of Mes-NiNc and Ph-NiNc molecular alignments. In-situ XRD experiment, computation, and simulation perspectives afforded prospective insertion and desertion behaviors of cations and anions.