The charge-ordered state in a quasi-two-dimensional organic superconductor β -(BEDT-TTF) 4 [(H 3 O)Ga(C 2 O 4 ) 3 ]·C 6 H 5 NO 2 has been investigated using 13 C NMR spectroscopy in a high magnetic field. Enhanced resolution of the high-field spectrum allows us to estimate the site charges in the low-temperature charge-ordered state below 8.5 K. The observed strong increase in the charge imbalance suggests that superconductivity appears on the electronic state with a strong charge modulation. From the NMR intensity ratio of signals from the charge-rich and charge-poor sites, we discuss a possible charge pattern with threefold modulation, which could be stabilized by the effects of electron-electron correlations. Unconventional superconductivity is frequently observed near the boundary of other ordered phases. In high-T c pnictides and heavy fermion superconductors, superconductivity appears next to an antiferromagnetic phase, and its mechanism is related to the critical fluctuations of the second-order phase transition. By analogy with antiferromagnetism near superconductivity, the charge-ordering (CO) transition near the superconducting (SC) phase would also be related to the SC pairing mechanisms. In fact, it has been suggested theoretically that the charge fluctuations can contribute to form Cooper pairs both in the context of cuprates [1] and layered molecular crystals [2]. As in most of materials the SC and CO transitions appear at very different temperatures, particular attention should be paid to rare examples where these transitions (and related energy scales) are close [3], to reveal experimentally the complex relationship, perhaps not only competition, between the CO and SC phases.Electronic charge localization is caused by a strong electron-electron interaction in half-filled or quarter-filled systems. The effects of on-site and off-site Coulomb interactions have been intensively investigated both from theoretical and experimental points of view [4][5][6]. In low-dimensional electronic systems, such as NbSe 3 [7] and organic conductor (TMTTF) 2 X (tetramethyltetrathiafulvalene) salts [8], the charge-density-wave (CDW) state with fractional charge localization is driven by Fermi surface instability. Although these systems show superconductivity under pressure, the CDW state of NbSe 3 is completely suppressed when superconductivity sets in [9], and in (TMTTF) 2 X a magnetic phase appears between the SC and CDW phases. Charge instability is also observed in quasi-two-dimensional organic conductors (BEDT-TTF) 2 X [bis(ethylenedithio)-tetrathiafulvalene] salts. In some BEDT-TTF salts, superconductivity appears directly after the suppression of the CO transition by applying chemical or mechanical pressure [10][11][12]. However, the CO transition temperature is much higher than the SC transition temperature T c [13,14], and the two phenomena thus appear * yihara@phys.sci.hokudai.ac.jp unrelated. In the BEDT-TTF salt with β -type molecular packing, β -(BEDT-TTF) 4 [(H 3 O)Ga(C 2 O 4 ) 3 ]·C 6 H 5 NO 2 (β -Ga)...