A new type of adsorbent, collagen fiber immobilized metal-ions(MICF) is prepared on the base of some metal-oxide salts and collagen fiber, and its adsorption behavior for removing fluoride in solution is investigated. It is suggested that ZrCF has good adsorption property for fluoride and in the pH range of 4.0-9.0, ion intensity has little effect on adsorption. In addition, the coexisting anions such as Cl -,NO -3 and SO 2-4 has no interference for adsorption. The ZrCF is described by means of SEM, surface charge and FTIR. It is obviously that Zr(Ⅳ) is uniformly impregnated on collagen fiber by means of SEM. The pHpzc increases up to 9.0 determined by the solid addition method. It is shown that the major adsorption mechanism is coordination exchange using the changes in pH value of solution and FTIR. In the adsorption procedure, the coordination complexation between Zr(Ⅳ)metal hydroxyl groups at the surface of ZrCF and fluoride occurs, and H + is discharged.