Zirconium- and hafinium-alkyldiylbisphosphonate multilayer films are prepared on modified gold and silicon substrates. The substrates are functionalized via 3-(hydroxydimethylsilyl) propanephosphonic acid and mercapto-3-butylphosphonic acid to yield a phosphonic acid surface. Mono- and multilayer films are then prepared by alternatively adsorbing metals such as Zr4+ and Hf4+, and alpha, omega-bis(phosphonic acids) from the aqueous solution. The characteristics of multilayer films were characterized by ellipsometry, x-ray reflectometry, AFM and surface plasmon resonance measurement.