An A-D-A triad compound comprising a tetrathiafulvalene (TTF) moiety and two pyridyl groups, py-TTF-py (1), has been Studied ill view of intramolecular charge transfer (ICT). The compound shows a sharp and multicolor change in different solvents and at different pH values, exhibiting good solvatochromism. The results of electronic absorption spectroscopy, cyclic voltammetry, and theoretical calculations confirm that there exists predominantly a monoprotonated A-D-A triad that displays a strong ICT effect, which is tunable as a function of pH. The equilibrium of protonation of 1 has been further studied by means of pH titration, and the result confidently Supports the conclusion that only one equivalent H+ combines with py-TTF-py in dilute Solution, even when excessive acid is added. However, unlike the state ill dilute solution, the crystal structure of the protonated 1 is a diprotonated A-D-A triad, (1 center dot 2H(+))center dot(CF3SO3-)(2)center dot H2O (2), that has been structurally characterized.