Adaptive mechanical behaviors in nature have inspired the development of synthetic adaptive composites, with those responsive to water particularly relevant for biomedical applications. Polymer nanocomposites containing cellulose nanocrystals (CNCs) are prime examples of water-responsive mechanically adaptive materials. Although CNCs are biobased, the matrixes of these composites are exclusively petroleum-based synthetic elastomers, in sharp contrast to their biological counterparts. In this work, we attempted to probe the possibility of using bioderived rubber(s) as the matrix to fabricate CNC-nanocomposite with water-responsive adaptive mechanical behaviors. Specifically, natural rubber (NR) and epoxidized natural rubber (ENR) were used as the composite matrixes. Our results show that the water-responsive sensitivity and reversibility of ENR composites is much more drastic than that of NR composites. This is attributed to the strong CNC-polymer interaction (hydrogen bonding) for ENR, which leads to better filler dispersion and the formation of an extra CNC-polymer network in addition to the CNC-CNC filler network present in the NR composite. The synergistic effect of the dual networks plays a key role in tuning the mechanical properties and water-responsive sensitivity for various potential biomedical applications. Our study further provides guidance to make use of renewable resources to produce high value added water-responsive nanocomposites.