------------------- GENERAL INFORMATION ------------------- 1. Title of dataset Supporting data for "Tunable Plasmonic Circular Dichroism of Hierarchical Chiral Assemblies" 2. Contact Principal Investigator Contact Information Name: Luis Liz-Marzán Institution: CIC biomaGUNE, University of Vigo Email: llizmarzan@cicbiomagune.es ORCID: https://orcid.org/0000-0002-6647-1353 3. Description of the project Plasmonic circular dichroism (PCD) is a powerful approach for enhancing chiroptical effects at the nanoscale with promising applications such as optical information processing, sensing, and catalysis. However, a key challenge remains in achieving both strong and tunable optical responses. While most strategies use either intrinsically chiral nanoparticles (NPs) or achiral NPs arranged into chiral assemblies, combining both offers a promising route to amplify chiral optical responses. Here, 4-fold-twisted gold nanorods (cGNRs) were assembled by depletion-induced self-assembly (DISA) into chiral superstructures with tunable PCD properties. By reducing cGNR helicity via chemical etching, we study how building block helicity affects hierarchical structure formation. Whereas static helical supercrystals were obtained on substrates upon evaporation-induced self-assembly (EISA), DISA allowed us to dynamically modulate the interparticle distance in solution from 13 ± 1.2 nm to 6.9 ± 1.0 nm. The assembly/disassembly process was found to be fully reversible, thereby enabling a modulation of the g-factor by 2 orders of magnitude with a switching rate of approximately 1 h. Beyond achieving high dissymmetry factors of 0.2, our approach establishes a reconfigurable PCD platform that is free from ligand exchange constraints and compatible with different NP shapes. Though response times remain too slow for optical computing, these findings are relevant for the development of optical modulators and memory devices based on dynamic chiral metafluids. 4. Description of the dataset The dataset regroup all the raw data used for the plotting, imaging and analysis of the paper. 5. Notes This dataset contains different folders corresponding to each figure in the main text and supporting information, collected by two different reserch groups involved in the project. Each folder contains different subfolders corresponding to the figures raw data, and and all the analysis performed. The numerical resuts are collected in Excel files. In general, - for the characterization of gold nanorods (kinetics, scattering), .dat files are provided - for each spectrum a .emi and .ser file is provided. - for the optical images a PNG file is provided.