This dataset contains supporting data for the manuscript entitled “Amino Acid Functionalised Perylene Bisimides for Aqueous Solution-deposited Electron Transporting Interlayers in Organic Photovoltaic Devices” The following data are included: Atomic force microscopy (AFM) thickness measurements - The directory names indicate the sample studied. The files (.dat) are repeat measurements of the depth profile of scratched films at different areas and are numbered 1 - 10. The data can be opened using text editor programmes such as notepad, wordpad or textedit. Atomic force microscopy topography - The directory names indicate the sample studied. The files (.flt) are the different measurements from the AFM scans where those with “SIG_T_B_FRW” indicate the the deflection data, “SIG_TM_AMPLITUDE_FRW” indicates the amplitude data, “SIG_TM_PHASE_FRW” indicates the phase data and “SIG_TM_TOPO_FRW” indicates the topography data. Only the topography data is presented in the manuscript. The data can be opened using commercial software, Bruker NanoAnalysis 1.5, or the open source software WSxM (http://www.wsxm.eu). Images generated from the topography measurements are also included and can be opened using image software e.g. Windows Photo Viewer, Photos. External quantum efficiency (EQE) measurements for solar cells - The directory names indicate the sample studied. The files (.xlsx) can determination of the external quantum efficiency of solar cells and the calculation of the short circuit current density using this data. The files can be opened using Microsoft Excel or other spreadsheet software Organic photovoltaic (OPV current-voltage (IV) data - The directory names indicate the sample studied based on the electron transport layers used. The files (.xls) are measurements of current-voltage profile of the fabricated solar cells either in the dark or under illumination with a solar simulator (labelled ‘light’). The files are numbered for measurements of different devices with the same structure. Transmittance data - The files (.txt) are measurements of transmittance of the films deposited on ITO/glass substrates. The The data can be opened using text editor programmes such as notepad, wordpad or textedit.