Elastomeric polysiloxane nanocomposites with elongations of >5000% (more than 3x greater than any previously reported material) with excellent shape recovery are presented. Highly deformable materials are desirable for the fabrication of stretchable implants and microfluidic devices. No crosslinking or domain formation is observed by a variety of analytical techniques, suggesting that their elastomeric behavior is caused by polymer chain entanglements.