The amino-tri-(methylenephosphonic acid) layers were adsorbed on the surface of AA6061 aluminum alloy for improving the lacquer adhesion and corrosion inhibition as a substitute for chromate coatings. The surface structure and characteristic of the amino-tri-(methylenephosphonic acid) layers on AA6061 aluminum alloy were investigated by means of XPS and ATR-FTIR analysis. The analyzed results showed that the amino-tri-(methylenephosphonic acid) adsorption layers adsorb on the surface of aluminium alloy via acid-base interaction in a bi-dentate conformation. After the amino-tri-(methylenephosphonic acid) layers were coated with epoxy resin, the layers showed good adhesive strength and favorable corrosion resistance in contrast to chromate coatings. The amino-tri- (methylenephosphonic acid) layers were adsorbed on the surface of AA6061 aluminum alloy for improving the lacquer adhesion and corrosion inhibition as a substitute for chromate coatings. The surface structure and characteristic of the amino-tri- (methylenephosphonic acid) layers on AA6061 aluminum alloy were investigated by means of XPS and ATR-FTIR analysis. The analyzed results showed that the amino-tri- (methylenephosphonic acid) adsorption layers on the surface of aluminum alloy via acid-base interaction in a bi-dentate conformation After the amino-tri- (methylenephosphonic acid) layers were coated with epoxy resin, the layers showed good adhesive strength and favorable corrosion resistance in contrast to chromate coatings.