1：Experimental Design and Method Selection:

The study utilized cyclic voltammetry (CV) and a simulation model to evaluate the electrochemical performance of nanostructured carbon electrodes. The electrodes were prepared by anodic electrodeposition of graphene quantum dot assemblies (HBC and CQD) onto conductive support.

2：Sample Selection and Data Sources:

The electrodes were made via electrodeposition from soluble precursors HPB and pre-CQD, synthesized as described in the Supporting Information.

3：List of Experimental Equipment and Materials:

Instruments used include a Bruker DPX and Avance III HD for NMR spectra, Bruker Ultraflextreme MALDI-Tof-Tof mass spectrometer for MALDI spectra, Ocean Optics spectrophotometer for UV-vis absorption spectra, Epsilon EC potentiostat and Gamry Interface 1010B and 1010E for electrochemical measurements, field emission SEM model JSM-6320F for SEM, and 300 kV JEM-3010 instrument for TEM.

4：Experimental Procedures and Operational Workflow:

The electrodes were characterized using UV-Vis absorption spectroscopy, infrared and Raman spectroscopy, grazing-incidence wide-angle x-ray scattering (GIWAXS), MALDI, and scanning and transmission electron microscopies (SEM and TEM).

5：Data Analysis Methods:

The voltammograms were simulated using a modification of a model developed by Bisquert and coworkers, assuming that the observed current predominantly arises due to the capacitive charging/discharging of the conductive film.