This dataset consists of in silico generated Orbitrap top-down proteomics spectra created using the FTMS simulator software (Spectroswiss). The simulated datasets are designed to evaluate false discovery rate (FDR) estimation in spectral deconvolution workflows. Protein sequences were used to generate MS spectra with varying resolution, noise, and charge characteristics. The dataset includes deconvolved TSV files and corresponding mzML spectra for each simulated run.