The vast majority of nanomaterials studied in light of their ability to transmit chirality to or amplify their chirality in a surrounding medium, constitute an achiral core with chirality solely installed at the surface by conjugation or encapsulation with optically active ligands. Here we present the inverse approach focusing on surface‐modified cellulose nanocrystals (CNCs) with core chirality at both the molecular and the morphological level to quantify transmission and amplification of core chirality through space using a host nematic liquid crystal (N‐LC) as reporter. We find that CNCs functionalized at the surface with achiral molecules, structurally related to the N‐LC, exhibit better N‐LC solubility, thereby serving as highly efficient chiral inducers. Moreover, functionalization with chiral molecules only marginally enhances the efficacy of helical distortion in the host N‐LC matrix, indicating the high propensity of CNCs to transfer chirality from an inherently chiral core.