Organic-inorganic hybrid light-emitting diodes (HyLEDs) consist of an organic emission layer in combination with at least one metal oxide charge injection layer, typically in an inverted structure. Low temperature, solution processing of metal oxide charge injection layers is one of the key factors in reducing the manufacture cost of HyLEDs. Herein, we report the use of composite materials, comprising conjugated polyelectrolytes (CPE) and zinc oxide nanoparticles (ZnO NPs), as the electron injection layer (EIL) in highly-efficient, green-light-emitting poly (9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) polymer LEDs that are carefully optimised for use in an inverted HyLED architecture for the first time. The composite CPE:ZnO EILs are processed via a room temperature, one-step, solution deposition and enable superior device performance relative to ZnO NPs on their own. We find that specifically, they (i) improve EIL morphology, reducing surface roughness as well as pin-hole size and density, (ii) induce a favourable vacuum level shift for electron injection by coordinate bonding between the CPE and ZnO constituents, and (iii) reduce interfacial quenching by passivation of ZnO chemical defects caused by oxygen vacancies. This work is also the first demonstration that blending ZnO NPs and CPE supports much faster electroluminescence turn-on times (~7.12 μs) than for traditional ZnO/CPE bilayer devices (~0.4 s) via ‘locking’ of the CPE mobile ions, as well as higher device performance. This demonstrates good suitability for display applications. After optimisation of the EIL composition and the thickness of the F8BT emissive layer, we achieve promising device efficiencies of 16.5 cd/A and 5.4 lm/W for devices with a 1.1 μm thick F8BT layer, which is particularly relevant for potential roll-to-roll fabrication. These results clearly demonstrate the potential that this organic-inorganic composite EIL material has for the realisation of cheap, scalable and highly efficient, printable HyLED devices.