Organic-semiconductor-based light-emitting diodes (OLEDs) are now attracting considerable interest due to their potential applications in flexible displays and solid-state lighting.[1] The key challenge for their technological exploitation is the development of device structures that i) exhibit improved environmental stability under operation, especially for flexible substrates, and ii) are able to emit with high efficiency at high luminance. [2][3][4] In terms of device stability, the use of highly reactive, lowwork-function metals such as barium or calcium as electron-injecting-layer (EIL) materials is a major concern for conventional OLED device architectures, since they easily degrade in the presence of oxygen and moisture. [5,6] As such, developing more-stable electrode systems and indeed new device architectures is critically important for the realization of both stable and efficient OLEDs. One recent approach is to use inorganic metal oxide films as charge-injection layers. Metal oxides are particularly attractive in this role due to their mechanical and electrical robustness, low-cost, visible-light transparency, excellent environmental stability, good charge-transport properties, and the controllability of their film morphology on nano-to micrometer length scales. Metal oxide films have been recently employed as hole (HIL) and electron (EIL) injection layers in hybrid organic-inorganic light-emitting diodes (HyLEDs). [7,8] The use of transparent metal oxide films as EILs is particularly attractive as it enables the use of opaque high-work-function metals, such as gold, for hole injection (with or without a separate HIL), yielding more-stable device architectures. Both titanium dioxide (TiO 2 ) [7,8] and zinc oxide (ZnO) [9] films have been recently investigated in polymer LEDs for use as EIL, and molybdenum trioxide (MoO 3 ) [7,9] as a HIL. Typically, dense thin films have been used, but we have also shown that nanostructured layers can be effective with the potential advantage of an enhanced injection current due to the convoluted contact area.[8] Devices reaching luminance levels of %6 500 cd m À2 have been reported for HyLEDs employing poly(9,9-dioctylfluorene-alt-benzothiadiazole) (F8BT) as an electroluminescent layer combined with ZnO and MoO 3 as EIL and HIL, respectively. [9] Whilst these studies demonstrate the attractiveness of this approach, further increases in luminance and efficiency are required before such devices can be considered commercially viable. Moreover, recent studies have also shown that the device function is dominated by hole injection, and that electron injection from the metal oxide EIL into the lowest unoccupied molecular orbital (LUMO) of the semiconducting polymer is a key limiting step.[10] For example, the relatively deep conduction-band level of TiO 2 (%3.8 eV below the vacuum level) compared to the LUMO (%3.5 eV) of F8BT may reduce the efficiency of electron injection. Therefore, it is important to design alternative EILs that enable efficient electron injection into t...