The dataset contains experimental data for the article entitled “1,2,5,6-Tetrathiocin as a scaffold for improved charge transport in double-cable oligothiophene systems”. This includes characterisation (NMR, mass spectrometry, elemental analysis) of molecules synthesised, UV/vis abosprtion, cyclic voltammetry, differential scanning calorimetry, thermal gravimetric analysis and bottom-gate, bottom-contact organic field-effect transistor measurements.