Updated project metadata. Peptide fragmentation spectra are routinely predicted in the interpretation of mass spectrometry-based proteomics data. Unfortunately, the generation of fragment ions is not well enough understood to estimate fragment ion intensities accurately. Here, we demonstrate that machine learning can predict peptide fragmentation patterns in mass spectrometers with accuracy within the uncertainty of the measurements. Moreover, analysis of our models reveals that peptide fragmentation depends on long-range interactions within a peptide sequence. We illustrate the utility of our models by applying them to the analysis of both data-dependent and data-independent acquisition datasets. In the former case, we observe a significant increase in the total number of peptide identifications at fixed false discovery rate. In the latter case we demonstrate that the use of predicted MS/MS spectra is equivalent to the use of spectra from experimentallibraries, indicating that fragmentation libraries for proteomics are becoming obsolete.