To reveal the nature of the zinc(II)-ion-induced ionochromic effect of bipyridine (bpy)-containing d-conjugated polymers, we proposed an electrostatic interaction mechanism to illustrate our recent experimental findings [ Tian, L., et al. J. Phys. Chem. B 2005 109 ( 15), 6944]. Our theoretical analysis was based on the semiempirical (INDO/2) calculation of spectral properties and electronic structures of difluorene-substituted bpy model compounds. Our calculations show that the zinc(II)-induced ionochromic effect can be attributed to the electrostatic interaction between the zinc( II) ion and the polymer. Zinc( II) ion acts as a positive point charge with varied charge quantities, which is responsible for the red-shifted absorption spectra compared with those of the metal-free compound. The counterion ionochromic effect of the zinc( II) ion is also discussed. The proposed mechanism is possibly applied to the ionochromic effect induced by other metal ions such as Cd(II) and Hg(II).