This dataset collection accompanies the paper titled “Fs-laser significantly enhances both above- and below-bandgap absorption in germanium”, published in Optical Materials Express. The experimental and computational methods used to generate these datasets are detailed in the original publication. The datasets include the values needed to recreate Figures 1b, 1c, 2b, 2c, 3a, 3b, 4c, and 4d, as well as raw Raman spectroscopy results used to compute Table 1. Each file is named according to the corresponding figure caption for easy identification, with headers distinguishing individual datasets. The file SEM.zip contains all raw SEM images for Figures 1a, 2a, and 4a. The images are named based on their figure captions and order of appearance in the paper. This content is licensed under CC BY 4.0. If using these datasets or figures, please ensure proper citation of the original paper: Liu, X., Gnatyuk, D., Halmela, J., Vähänissi, V., & Savin, H. (2024). Fs-laser significantly enhances both above- and below-bandgap absorption in germanium. Optical Materials Express, 15(2). https://doi.org/10.1364/OME.545692