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We report the influence of surface morphology and charge of alginate/chitosan (ACA) microcapsules on both the amount of adsorbed protein and its secondary structural changes during adsorption. Variations in surface morphology and charge were controlled by varying alginate molecular weight and chitosan concentration. Plasma fibrinogen (Fgn) was chosen to model this adsorption to foreign surfaces. The surface of ACA microcapsules exhibited a granular structure after incubating calcium alginate beads with chitosan solution to form membranes. The surface roughness of ACA microcapsule membranes decreased with decreasing alginate molecular weight and chitosan concentration. Zeta potential measurements showed that there was a net negative charge on the surface of ACA microcapsules which decreased with decreasing alginate molecular weight and chitosan concentration. The increase in both surface roughness and zeta potential resulted in an increase in the amount of Fgn adsorbed. Moreover, the higher the zeta potential was, the stronger the protein-surface interaction between fibrinogen and ACA microcapsules was. More protein molecules adsorbed spread and had a greater conformational change on rougher surfaces for more surfaces being available for protein to attach.