A phenomenological modeling approach was developed to try to understand the reinforcing mechanism of starch nanocrystals in a nonvulcanized natural rubber matrix. Natural rubber was not cross-linked to maintain the biodegradability of the biosourced materials. Nonlinear dynamic mechanical experiments highlighted the significant reinforcing effect of starch nanocrystals and the presence of the Mullins and Payne effects. Two models were used to predict the Payne effect considering that either filler filler (Kraus model) or matrix filler (Maier and Goritz model) interactions are preponderant. The use of the Maier and Goritz model demonstrated that phenomena of adsorption and desorption of NR chains on the filler surface governed nonlinear viscoelastic properties, even if the formation of a percolating network for filler contents > 6.7 vol % was evidenced by the Kraus model.