Basic yellow has shown great application in chemical and biological field as a dye. Ethanol-based basic yellow solution is used to enhance the deposit of superglue-developed fingermarks in forensic science. However, the potential applications of basic yellow doped nanomaterials in forensic science, latent fingermark development in particular, were still unclear. In this study, we have succeeded in trapping basic yellow in silicon dioxide-based nanomaterials, doped aerogels, using the sol–gel method. We have tested the detection for latent fingermarks left under different conditions. The results indicated that the basic yellow doped aerogels applicable for latent fingermark development on various forensic relevant materials, including metal foil, glass, plastic, and paper, etc. The procedure of preparation and fingermark labeling results of these new basic yellow doped nanomaterials are presented in this study.