Genome mining has become an invaluable approach in aiding the discovery of peptide natural products; a large and diverse group of potentially bioactive molecules. Here we propose nanoDESI based MS/MS networking to map the searchable molecular universe of a large number of strains. The organization of the molecular universe via MS /MS networking enables molecular family guided genome mining to connect NRPS molecular families produced by unsequenced organisms to candidate gene cluster families found in publicly available genome databases. As proof-of- principle, we collected nanoDESI MS/MS data on 42 bacilli and 17 pseudomonads and used molecular MS/MS networking to identify the peptidic products through generation of amino acid sequence tags from the MS/MS data. Furthermore, we use these studied dataset to identify unknown molecules from unsequenced microbes