The　interaction　of　low-energy　electrons　(LEEs)　with　DNA　plays　a　significant　role　in　the　mechanisms　leading　to　biological　damage　induced　by　ionizing　radiation,　particularly　in　radiotherapy,　and　its　sensitization　by　chemotherapeutic　drugs　and　nanoparticles.　Plasmids　constitute　the　form　of　DNA　found　in　mitochondria　and　appear　as　a　suitable　model　of　genomic　DNA.　In　a　search　for　the　best　LEE　targets,　damage　was　induced　to　plasmids,　in　thin　films　in　vacuum,　by　6,　10,　and　100　eV　electrons　under　single　collision　conditions.　The　yields　of　single-　and　double-strand　breaks,　other　cluster　damage,　isolated　base　lesions,　and　crosslinks　were　measured　by　electrophoresis　and　enzyme　treatment.　The　films　were　deposited　on　oriented　graphite　or　polycrystalline　tantalum,　with　or　without　DNA　autoassembly　via　diaminopropane　(Dap)　intercalation.　Yields　were　correlated　with　the　influence　of　vacuum,　film　uniformity,　surface　density,　substrates,　and　the　DNA　environment.　Aided　by　surface　potential　measurements　and　scanning　electron　microscopy　and　atomic　force　microscopy　images,　the　lyophilized　Dap-DNA　films　were　found　to　be　the　most　practical　high-quality　targets.　These　studies　pave　the　way　to　the　fabrication　of　LEE　target-films　composed　of　plasmids　intercalated　with　biomolecules　that　could　mimic　the　cellular　environment;　for　example,　as　a　first　step,　by　replacing　Dap　with　an　amino　acid.　©　2022　American　Chemical　Society.