Achieving scalable fabrication with precise control of chiroptical properties in chiral plasmonic materials remains challenging.We present a new family of engineered chiroptical composites comprising linearly assembled gold nanoparticle arrays integratedwith cholesteric self-assembled cellulose nanocrystals (CNCs). Aqueous CNC suspensions are cast onto pre-assembled achiralplasmonic nanoparticle arrays via evaporation-induced transfer imprinting lithography, yielding centimeter-scale hybrid filmswith custom-tailored chiroptical responses. During drying, CNCs co-assemble with the gold nanoparticles at the interface,preserving the array’s linear arrangement and keeping it isolated from the overlying cholesteric CNC layers. This configurationcombines the linear dichroism of the plasmonic array with the linear birefringence of the CNC matrix, producing strong andtunable plasmonic circular dichroism at the surface lattice resonance, reaching 1217 ± 51 mdeg with a dissymmetry factor of –0.19± 0.02. Our approach provides a sustainable platform for engineering multifunctional chiral plasmonic materials with potentialapplications in optical sensing, photonic devices, and chiral biointerfaces.