The successful incorporation of an organic chromophore with highly polariza
ble lead iodide chains in an organic-inorganic hybrid is revealed in this c
ommunication. The synthesis, structure, and preliminary studies of the line
ar and nonlinear optical (NLO) properties of the compound are divulged. The
synergism exhibited between polarizable inorganic polymers and hyperpolari
zable organic molecules provides a route to new multi-functional NLO materi
als.