A series of mono- and polynuclear ferrocenylthiosemicarbazone complexes were prepared via nucleophilic substitution reactions of various amine scaffolds with a ferrocenyl dithiocarbamate. The dithiocarbamate was prepared via a Schiff base condensation reaction. The compounds were characterised using various spectroscopic and analytical techniques including Nuclear Magnetic Resonance (NMR) and Infrared (IR) spectroscopy, mass spectrometry and elemental analysis. The ferrocenyl dithiocarbamate and thiosemicarbazone compounds were screened for their preliminary antimicrobial activity against the H37Rv strain of Mycobacterium tuberculosis and the chloroquine-sensitive (CQS) NF54 strain of Plasmodium falciparum. Against M. tuberculosis, the compounds displayed moderate to low activity. The mononuclear and octanuclear complexes were the most active, exhibiting similar MIC values. All compounds displayed moderate activity in the antiplasmodial screening. The mononuclear and trinuclear complexes exhibited enhanced activity compared to the complexes with higher nuclearity.