Novel chitosan/pectin/gum Arabic polyelectrolyte complex (PEC) solutions and membranes with variouscompositions were prepared for biomedical applications. The appearance of the PEC solutions, eitherclear or turbid, was process-dependent and depended on how the three components were dissolvedand mixed. The addition of gum Arabic to the chitosan and pectin significantly decreased the viscositiesof the resultant PEC solutions due to the formation of globe-like microstructures that was accompa-nied by network-like microstructures and other molecular entanglements. The mechanical strength andhydrophilicity of the PEC membranes manufactured from the PEC solutions, especially for a weight ratio of84/8/8 (chitosan/pectin/gum Arabic), were enhanced compared to pure chitosan membranes. Moreover,the use of the 84/8/8 PEC membranes as a drug carrier exhibited steady and fairly complete release of adrug (insulin) for 6 h. Based on these promising results, the chitosan/pectin/gum Arabic PEC membraneshave great potential in controlled drug release applications.