In this Article, we study the binary surface interactions of 1,2-dimyristoyl-rac-glycero-3-O-(N(alpha)-acetyl-L-arginine) hydrochloride (1414RAc) with 1,2-dipalmitoyl-sn-glycero-3-phosphatidylcholine (DPPC) on 0.1 M sodium chloride solutions. 1414RAc is a novel monocationic surfactant that has potential applications as an antimicrobial agent, is biodegradable, and shows a toxicity activity smaller than that of other commercial cationic surfactants. DPPC phospholipid was used as a model membrane component. The dynamic surface tension of 1414RAc/DPPC aqueous dispersions injected into the saline subphase was followed by tensiometry. The layer formation for the mixtures is always accelerated with respect to DPPC, and surprisingly, the surface tension reduction is faster and reaches lower surface tension values at surfactant concentration below its critical micellar concentration (cmc). Interfacial dilational rheology properties of mixed films spread on the air/water interface were determined by the dynamic oscillation method using a Langmuir trough. The effect of surfactant mole fraction on the rheological parameters of 1414RAc/DPPC mixed monolayers was studied at a relative amplitude of area deformation of 5% and a frequency of 50 mHz. The monolayer viscoelasticity shows a nonideal mixing behavior with predominance of the surfactant properties. This nonideal behavior has been attributed to the prevalence of electrostatic interactions.