The use of scalable technology for the fabrication of stretchable-transistor active matrixes can promote rapid growth in the development of intrinsically stretchable displays. [11] However, since the stretchability of polymer light-emitting diodes (PLEDs) is limited, [12] intrinsically stretchable active-matrix organic light-emitting diodes (is-AMOLEDs) based on is-PLEDs have not yet been realized.The development of is-PLEDs is hindered primarily by the limited stretchability of the emissive layer and the chargeinjection interlayers. [13] Unlike in the case of stretchable transistors and other stretchable electroluminescent devices, [14] the development of stretchable PLEDs is also hindered by constricted energy-level alignment [15][16][17] and the rigorous requirement of injecting balanced charge to the emissive layer. [18,19] Furthermore, it is difficult to simultaneously achieve desirable charge transportability, appropriate energy-level alignment, and increased stretchability in the emissive layer of an is-PLEDs. Unlike in the case of intrinsically stretchable polymer semiconductors, [20][21][22] techniques for the design and synthesis of novel intrinsically stretchable luminescent polymers are currently being studied; [23][24][25] novel design concepts are needed to achieve improved luminescent and stretchable properties simultaneously. Moreover, the 3D vertical channels for charge transport throughout the emissive layer of a PLED are indispensable, unlike the quasi-2D horizontal channels field-effect transistors. Therefore, the nanoconfinement-elastomer-matrix strategy [26] and nanowire-polymer-matrix-assembly strategy, [27] which are extensively used for stretchable field-effect transistors, are not as effective for traditional luminescent polymers. An emissive polymer typically exhibits a significant decrease in mobility after the addition of a secondary elastomer component, [28] which results in an increase in the interchaincharge-transfer energy barrier; this is because the secondary elastomer acts as an interchain spacer in the emissive polymer after blending. Emissive polymer semiconductors have poor self-assembly properties due to which charge transportability significantly decreases after elastomer addition. Thus, there is a tradeoff between stretchability and mobility. PLEDs based onThe emergence of wearable technology can significantly benefit from electronic displays fabricated using intrinsically stretchable (is-) materials. Typically, an improvement in the stretchability of conventional light-emitting polymers is accompanied by a decrease in charge transportability, thus resulting in a significant decrease in device efficiency. In this study, a self-assembled 3D penetrating nanonetwork is developed to achieve increased stretchability and mobility simultaneously, based on high-molecular-weight phenylenevinylene (L-SY-PPV) and polyacrylonitrile (PAN). The mobility of L-SY-PPV/ PAN increases by 5-6 times and the stretchability increases from 20% (pristine L-SY-PPV film) to 100%. A high current eff...