The widespread use of renewable nanomaterials has been limited due to poor integration with conventional polymer matrices. Often, chemical and physical surface modifications are implemented to improve compatibility, however, this comes with environmental and economic cost. This work demonstrates that renewable nanomaterials, specifically cellulose nanocrystals (CNCs), can be utilized in their unmodified state and presents a simple and versatile, one-step method to produce polyamide/CNC nanocomposites with unique Janus-like properties. Nanocomposites in the form of films, fibers, and capsules are prepared by dispersing as-prepared CNCs in the aqueous phase prior to the interfacial polymerization of aromatic diamines and acyl chlorides. The diamines in the aqueous phase not only serve as a monomer for polymerization, but additionally, adsorb to and promote the incorporation of CNCs into the nanocomposite. Regardless of the architecture, CNCs are only present along the surface facing the aqueous phase, resulting in materials with unique, Janus-like wetting behavior and potential applications in filtration, separations, drug delivery, and advanced fibers.