Rubber materials are the key components of flexible optoelectronic devices, especially for the light-emitting diodes based on arrays of inorganic nanowires (NWs). This paper reports on polydimethylsiloxane-graft-polystyrene (PDMS-St) as a new flexible substrate of GaP NW array structures. The NWs were encapsulated by the newly introduced G-coating method to substitute the inefficient mainstream spin-coating. To further exploit the flexibility and the stretchability of the NW/PDMS-St structures, the ferrocenyl-containing polymethylhydrosiloxane was synthesized and successfully used as an electrode for the NWs. In order to make an alternative highly efficient transparent electrode, a new application of conductive single-walled carbon nanotubes was demonstrated. The novel materials and methods demonstrated unsurpassed mechanical stability of the fabricated flexible electronic devices.