Macroscopic superlattices of tin-doped indium oxide (ITO) nanocrystals (NCs) are prepared by self-assembly at the air/liquid interface followed by simultaneous ligand exchange with the organic semiconductor copper 4,4',4″,4‴-tetraaminophthalocyanine (Cu4APc). By using X-ray photoelectron spectroscopy (XPS), grazing-incidence small-angle X-ray scattering (GISAXS), and ultraviolet-visible-near-infrared (UV-vis-NIR) spectroscopy, we demonstrate that the semiconductor molecules largely replace the native surfactant from the ITO NC surface and act as cross-linkers between neighboring particles. Transport measurements reveal an increase in electrical conductance by 9 orders of magnitude, suggesting that Cu4APc provides efficient electronic coupling for neighboring ITO NCs. This material provides the opportunity to study charge and spin transport through phthalocyanine monolayers.