In the present study, tissue responses of two types of three-dimensional titanium fiber structure, namely, titanium web (TWe) and titanium wire (TWi), were evaluated for external and internal bone augmentation, respectively. TWe was produced by sintering intertwined thin titanium fibers. TWi was produced by interweaving thin titanium fibers without a sintering process. The mechanical strength was superior in TWe and the formability was superior in TWi. As surface modifications of TWe and TWi, both CA coating using a molecular precursor method and immobilization of cell-adhesive protein, collagen and fibronectin, using the tresyl chloride-activated method were employed. TWe materials were implanted under the periosteum of rat calvaria to evaluate the external bone augmentation. TWi materials were implanted into the bone defect of rabbit femoral condyle to evaluate the internal bone augmentation. After 4 and 8 weeks for rat experiments with TWe materials and 12 weeks for rabbit experiments with TWi materials, new bone formation inside the porous area of the fiber structure was histologically evaluated. The bone formation rate (BFR) and the vertical bone augmentation rate (VBR) were also histomorphometrically analyzed. BFR and VBR of CA-coated TWe and TWi were significantly higher than those of non-coated TWe and TWi, respectively, for rat external and rabbit internal bone augmentation (p<0.05). BFR of collagen-or fibronectin-immobilized TWi was significantly higher than for non-coated TWi for rabbit internal bone augmentation (p<0.05), but not for rat external bone augmentation (p>0.05). In conclusion, it is suggested that surface-modified three-dimensional titanium fiber structure is a good candidate as a three-dimensional scaffold for regenerative medicine.