Amphiphilicity and cationicity are properties shared between antimicrobial peptides and proteins that catalyze biomineralization reactions. Merging these two functionalities, we demonstrate a reaction where a cationic antimicrobial peptide catalyzes self-biomineralization within inorganic matrices. The resultant antimicrobial peptide nanoparticles retain biocidal activity, protect the peptide from proteolytic degradation, and facilitate a continuous release of the antibiotic over time. Taken together, these properties demonstrate the therapeutic potential of self-synthesizing biomaterials that retain the biocidal properties of antimicrobial peptides.