The phase transition of tetramethylpyrazine-chloranilic acid (1:1) was studied by 35 Cl NQR measurements. The frequency splits into a doublet below T c = 83.0 ± 0.5 K. The averaged frequency of 36.98 MHz at 77 K suggests an electrically neutral electronic state of the chloranilic acid molecule, that is, no proton transfer between the acid and base molecules. An enhancement of the relaxation rate was observed at T c : it is presumably due to critical slowing down of a hydrogen motion in the one-dimensional hydrogen bond network. The excitation of a hightemperature hydrogen motion at T > 250 K is also suggested by the steep decrease of T 1 observed above 250 K. From the slope of the Arrhenius plots, an activation energy of 35 kJ mol −1 is calculated for the motion.