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We present $^{127}$I nuclear quadrupole resonance spectra and nuclearrelaxation of $\alpha$-(BEDT-TTF)$_2$I$_3$ that undergoes a charge-orderingtransition. Only one of the two I$_3$ anion sites shows a significantdifferentiation in the electric field gradients across the first-ordertransition. The charge modulation only in the BEDT-TTF layers can notreproduce; instead, an anion-donor interaction accompanied by hydrogen bondingis necessary. The dominating source for the nuclear relaxation is the locallibration of the I$_3$ anions, but an anomalous peak is detected just below thetransition, as observed by $^{13}$C NMR.

Role of hydrogen bonding in charge-ordered organic conductor $\alpha$-(BEDT-TTF)$_2$I$_3$ probed by $^{127}$I nuclear quadrupole resonance