We have studied nanostructured (NS‐) thin‐film electroluminescent (TFEL) devices utilizing the ZnS nanocrystals (NCs) with the mean crystal sizes of ca. 2–4 nm doped with activator‐ions. As compared to the conventional TFEL device, we have achieved a remarkable reduction in the operation voltages by >100 V0–p. Moreover, toward full‐color emissions, EL emissions of three primary colors, i.e., red, green, and blue have been derived from Mn2+, Tb3+, and Tm3+ ions, respectively. In this article, we review the studies on the fundamental properties of ZnS NCs as well as the device performance of the NS‐TFEL devices. We also discuss the excitation mechanisms of the activator‐ions in the ZnS NCs. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)