The doping of transition metal ions, such as Cu+ and Mn2+ into a quantum dot (QD) host is one of the useful strategies in tuning its photoluminescence (PL). This study reports on a two-step synthesis of Cu-doped InP QDs double-shelled with ZnSe inner shell/ZnS outer shell. As a consequence of the double shelling-associated effective surface passivation along with optimal doping concentrations, Cu-doped InP/ZnSe/ZnS (InP:Cu/ZnSe/ZnS) QDs yield single Cu dopant-related emissions with high PL quantum yields of 57–58%. This study further attempted to tune PL of Cu-doped QDs through the variation of InP core size, which was implemented by adopting different types of Zn halide used in core synthesis. As the first application of doped InP QDs as electroluminescent (EL) emitters, two representative InP:Cu/ZnSe/ZnS QDs with different Cu concentrations were then employed as active emitting layers of all-solution-processed, multilayered QD-light-emitting diodes (QLEDs) with the state-of-the-art hybrid combination of organic hole transport layer plus inorganic electron transport layers. The EL performances, such as luminance and efficiencies of the resulting QLEDs with different Cu doping concentrations, were compared and discussed.