The folder named “DLS” contains files with raw DLS data, used to calculate the critical micelle concentrations presented in the manuscript and ESI. The file name indicates the isomeric state and identity/structure (carbon tail length, spacer length) of each AzoTAB. For CMC determination, the count rate for a fixed attentuator distance (column 9 of the file) was the variable plotted against concentration. Each concentration has three measurements, the average value was taken.

The folder labelled “Surface Tension” contains surface tensiometry measurements were performed on a Kibron EZ-Piplus surface tensiometer using a DyneCups plastic cuvette (3 mL) and a DyneProbe ring. The obtained data were recorded on AquaPiPlus software and were averaged from 5 runs for each sample. Millipore water was used as a reference sample. Each file contains the AzoTAB concentration in water (X), the surface tension measured (Y) and error on the surface tension measurement (Y error).

SANS data are available in Folder "Figure 4" for the trans isomers and "Figure 5" for the cis isomers. Each filename provides the isomeric state, identity and concentration (in D2O) of each AzoTAB. The files contain q range (X), intensity as a function of q (Y) and error on intensity (Y error).

Cryo-SEM data are available in the folder "Figure 6"as .tif files. The file name contains the isomeric state and identity of the AzoTAB.

Characterisation data for the final AzoTABS are available in the folders "FTIR", "Mass Spectra" and "NMR". The NMR data subfolder "1" provides proton NMR while the subfolder "13" provides carbon NMR. These folders can be directly dragged and dropped/opened with the relevant NMR software (e.g MestreNova or TopSpin).

Folder S16 provides data for the effect of photoisomerization on the UV/Vis absorption spectra of C4AzoOC6TAB in water and below the CMC. Data provided is absorbance as a function of wavelength for the trans and cis forms.

Folder S24 provides data for the absorption spectra of C6AzoOC4TAB measured before (red line) and after (black line) illumination at λ = 365 nm. Data provided is absorbance as a function of wavelength for the trans and cis forms.

Folder S26 provides data histograms representing the size distribution for trans and cis-C8AzoOC2TAB obtained from Cryo-SEM images. Sizes were measured using the ImageJ software.