This dataset contains supporting data for the manuscript entitled “1,2,5,6-Tetrathiocin as a scaffold for improved charge transport in double-cable oligothiophene systems” The manuscript describes studies of 4 main compounds - 3T-TTC, 5T-TTC, EH-5T-TTC and 7T-TTC. Corresponding data are labelled in filenames and directories. Data on the synthesis of EH-5T-TTC has previously been published (https://doi.org/10.1039/C9SE00343F). The following data are included: Atomic force microscopy (AFM) - The topography data from AFM scans are saved as Files with a three digit extension e.g. xxx.001. The data can be opened using the open source software WSxM (http://www.wsxm.eu). Files with .stp extension or a three digit extension e.g. xxx.001 can be opened using WXsM. Cyclic voltammetry data - Text (.txt) files can be opened using text editor software such as Notepad or Wordpad. Left hand column is potential values (volts) and right hand column is current (amps). DSC and TGA - Includes differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) results. DSC data are saved as (.pdf) PDF files can be opened using PDF reader software such as Adobe Acrobat. .001 file extension is also included, this data can be opened using commercial software from TA Instruments. TGA data are saved as .csv file and can be opened using Microsoft Excel or other spreadsheet software Elemental Analysis - Images of spectra from elemental analysis service at University of Strathclyde. PDF files can be opened using PDF (.pdf) reader software such as Adobe Acrobat Mass Spectrometry - Images of spectra from mass spectrometry analysis service at University of Strathclyde. PDF files can be opened using PDF (.pdf) reader software such as Adobe Acrobat NMR spectroscopy data - 1H and 13C NMR spectra can be opened with commercial softwareTopSpin software which can be downloaded from Bruker (free for academic license) or MestreNova Organic field-effect transistor measurement data - The files (.xls) aand (.xlsx) are measurements of output characteristics and transfer plots for bottom-gate, bottom-contact organic field-effect transistors. Directory names are used to differentiate between different optimisation steps (compound, solvent used for deposition, self-assembled monolayer used (SAM), annealing temperature) as detailed in the manuscript. These files can be opened using Microsoft Excel or other spreadsheet software. UV-vis spectroscopy data - Text (.txt) files can be opened using text editor software such as Notepad or Wordpad.