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The influence of poly(ε-caprolactone) (PCL) grafts on the rheology and crystallization behavior of nanocomposites based on PCL and cellulose nanocrystals (CNC) both under quiescent and shear conditions is investigated. Under quiescent conditions, the grafted nanocrystals have high nucleation efficiencies. Under the influence of shear, the non-grafted nanocrystals were, however, more efficient in orienting the polymer chains and accelerating the flow-induced crystallization. The addition of large amounts of grafted material decreases the viscosity of the composites and thereby also the efficiency of shear-induced orientation.