Description of the dataset belonging to the manuscript entitled: Molecularly thin, energy-converting and self-healing membranes with macroscopic areas at water-water interfaces Authors: Christian C. M. Sproncken, Peng Liu, Justin Monney, William Stuart Fall, Carolina Pierucci, Philip B. V. Scholten, Brian van Bueren, Marcos Penedo, Georg Ernest Fantner, Rik Wensink, Ullrich Steiner, Christoph Weder, Nico Bruns, Michael Mayer and Alessandro Ianiro Corresponding authors: Alessandro Ianiro (alessandro.ianiro@unifr.ch) and Michael Mayer (michael.mayer@unifr.ch) Address: University of Fribourg, Adolphe Merkle Institute, Chemin des Verdiers 4, 1700 Fribourg, Switzerland. All data was collected from 2021 to October 2023 in Fribourg and Lausanne, Switzerland, and Paris, France. Methods for data collection, including instrument types and settings, are available from the main text and supplementary information of the related publication. List of used variables and their abbreviations: C = capacitance of the membrane R = resistance of the membrane P = resistivity of the membrane A = area of the membrane D = membrane diameter r = membrane radius d = membrane thickness V = voltage, potential I = current RIU = refractive index units subnotation SPEC is for specific, meaning normalized by area Data file descriptions in alphabetical order, excluding zipped folders: AFM.gwy is the raw height image used in the main text figure and AFM.py is script used to do the processing of the curve. The AFM area file contains the raw data for the curve. Data_read_Elements.py is the Python code used to analyze current recordings while applying a (triangular or sinusoidal) voltage wave to obtain the membrane thickness and resistance. Membrane_selfhealing_221117.csv contains the current traces of two membranes formed with a 4.5 mm diameter using the toluene displacement method, while being pierced with the Ag/AgCl wire electrode, causing current to saturate, which then restores to near-zero when the electrode is removed from the membrane. Note that the additional noise is due to the Faraday cage being open in order to move the electrode up and down. MembraneSPM-square-final__230224_003_NCM Phase_Forward.txt contains the XYZ data, where Z is the phase angle (degrees), of the surface probe micrograph taken from a membrane, assembled with the toluene displacement method and deposited onto a silicon wafer. MembraneSPM-square-final__230224_003_Z Height_Forward.txt contains the XYZ data, where Z is the height (nm), of the surface probe micrograph taken from a membrane, assembled with the toluene displacement method and deposited onto a silicon wafer. MembranepropertiesLarge.csv contains the properties determined via electrical measurements for membranes assembled at the ATPS interface using the toluene displacement method. Osmolality-matching.csv contains the measurement of osmolality for PEO in NaCl and Dextran in KCl solutions to determine the NaCl concentration needed in the PEO solution to match the osmolality of the DEX/KCl solution. ResistivityvsArea.csv contains the data used to plot the resistivity of membranes assembled at the ATPS interface using the toluene displacement method versus the membrane area. Sims_input is the LAMMPS input file for the simulation, while Sims_co is the file containing the final coordinates. Voltage-OC-device#.csv (where # is 1-4) contain the measured voltages with the source meter from four different 4-membranes-in-series devices in open circuit and under various loads, as well as the associated currents. Data file descriptions of the contents of zipped folders in alphabetical order: NMRdata contains the proton nuclear magnetic resonance spectra of synthesized block copolymers and their precursors, with the file name indicating the name of the compound. Syntheses are described in detail in the supplementary information of the related publication. PHMA-membranes contains the capacitances and therefrom calculated bilayer thicknesses of membranes made with the toluene displacement method, consisting of copolymers with poly(hexylmethacrylate) as hydrophobic block and its comparison to membranes based on poly(dimethylsiloxane). PlanarBilayerMembranes contains the properties (capacitance, thickness, resistance) of membranes, composed of PDMS-b-PEO, PDMS-b- PDMAEMA and a mixture of the two, measured through electrical methods with diameters ranging between 100 and 500 micrometers. SEC-data contains the size exclusion chromatograms (RIU versus time) for all synthesized copolymers and precursors. Valinomycin-IV-curves contains the current-voltage recordings for membranes (r = 2.25 mm) with various concentrations of valinomycin, expressed in mol % with respect to block copolymer concentration in toluene, formed via the toluene displacement method. Positive electrode was in the KCl-containing phase. Valinomycin-small-membranes contains the current voltage recordings for (r = 0.05 mm) with various concentrations of valinomycin, expressed in mol % with respect to block copolymer concentration in toluene, formed via the planar bilayer folding method. Positive electrode was in the KCl-containing phase.