AbstractRubber nanocomposites exhibit strain softening under large‐amplitude oscillation shear and large‐strain cyclic tension while the softening behaviors are hard to regulate in industry. Herein, an oligomer deep eutectic solvent (DES) synthesized from polyethyleneglycol and tetrabutylammonium bromide is used to mediate the vulcanization and softening behaviors of natural rubber (NR) gums and their nanocomposites. The results show that DES could accelerate NR vulcanization and improve crosslinking density. For the hydrophilic silica nanocomposites, DES could greatly reduce tanδ and weaken weak strain overshoot accompanying Payne and lower percentages damping accompanying Mullins effects. The effects in nanocomposites filled with hydrophilic/hydrophobic silica and carbon black are investigated and compared. The investigation provides a new way for tailoring elasticity and dissipation of vulcanizate nanocomposites filled with hydrophilic silica.