This dataset contains raw data used in the manuscript "Chemical Lithiation Reveals the Structures of Conjugated Tetralithium Dicarboxylates ". The dataset contains raw data for solid-state NMR spectra, powder X-ray diffraction patterns, crystal structures, DFT input and output files, Electrochemical data, EPR spectra and SEM images used in the manuscript. The data is in various formats and can be viewed using proprietary and free software - more details are given in the Readme file. This work forms part of the NEXGENNa project funded by the Faraday Institution, with full funding details given at the end of the associated manuscript.