Fabrication of crystalline organic tetracyanoquinodimethane (TCNQ) thin films using an ionized-cluster-beam (ICB) deposition method was investigated. Transmission electron microscopy (TEM) and Small Angle X-ray Scattering (SAXS) measurements of the films were performed. At a set of critical parameters of the ICB deposition, a single crystalline TCNQ thin film was obtained. Moire fringes of the crystalline TCNQ thin films were found in the TEM analysis of the ICB deposited film.