A hexadecane-1,1-bisphosphonic acid monolayer was grafted on the surface of muscovite mica via a simple selfassembled method. The result of AFM showed that the height of the bisphosphonate SAMs was about 2.40 nm, corresponding to both monolayer-like coverage and the hydrocarbon chain length. TOF SIMS indicated that the reaction between bisphosphonic acid and silicon was took place on the surface of mica substrate. It can be proved from IR, AFM, XPS, and TOF SIMS that the alkylbisphosphonate SAM was bonded to the mica with the mode of double-tridentate attachment. In addition, organobisphosphonate SAM possessed excellent orderliness and stability, which provides a theoretical basis for its efficient application in the field of organic modification.