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Poly(phenylene ethynylene) (PPE)-based cationic conjugated polyelectrolytes (CPEs) and cationic phenylene ethynylene oligomers (OPEs) exhibit broad-spectrum antimicrobial activity and one of their main targets is believed to be the bacterial cell wall and membrane. This review focuses on recent progress made in elucidating the membrane perturbation mechanism of these antimicrobial molecules. We first review the membrane action models proposed for naturally occurring antimicrobial peptides (AMPs) because the membrane activities of CPEs and OPEs and AMPs are believed to be mediated by the same physical and chemical driving forces. An overview of the current research progress on the interactions between CPE and OPE compounds and model membranes is then presented, including main parameters controlling the membrane activity of these synthetic antimicrobial compounds. Combined with …