A new strategy was developed to prepare disorderly exfoliated nanocomposites, in which a soft siloxane surfactant with a weight-average molecular weight (H,,) of 1900 was adopted to modify the clay. The modified clay slurry was then mixed with silicone rubber by hand, and exfoliation was achieved. The proposed mechanism thereof was verified by TEM and XRD. The physical entanglement of the soft siloxane surfactant plays a vital role in the diffusion and intercalation of the matrix molecules during the compounding of the slurry-polymer mixture. This simple method is applicable to other silicone-based materials reinforced by clay.