Fingermarks are a still primary form of evidence in any crime (and are particularly important in major crimes). This collection refers to a project funded by DASA UK regarding the engineering of a TRL 6 software the specific processing of crime scenes fingermark through of Matrix Assisted Laser Desorption Ionisation Mass Spectrometry Imaging (MALDI MSI). The software integrates artificial intelligence for the smart and fast provision of the highest quality fingermark images for National Database comparison and match, offering an increased likelihood of suspect identification. The Collection specifically includes: a) project background, aims, objectives and hypotheses; b) the machine learning algorithm (code) developed to assign a Scotland Yeard grade to each MALDI MS image of fingermark recovered; c) detailed information on the scripts, files, and folders used, along with the file structure and naming conventions (data level documentation (pdf). The metadata file (.xls) contains two sheets: one for the code scripts and another for the images.