Hydroxyapatite (HA) nanoparticle - collagen composite materials with various HA/collagen weight ratios were prepared from HA/collagen dispersions using the solution deposition and electrospinning with static or rotating collectors. The composites with nanoparticle HA to collagen weight ratio of 80:20 can be easily prepared in the solution deposition approach, whereas in the electrospun fibrous composites it was possible to reach a maximum HA/collagen weight ratio of 30:70 while maintaining a good fibrous structure. The structure, surface morphology, and nanoindentation properties of these nanoparticle HA/collagen composites with different microarchitectures were investigated. The values from 0.2 GPa to 20 GPa for nanoindentation Young's modulus and from 25 MPa to 500 MPa for hardness, were obtained depending on the fabrication technique, composition, and microarchitecture of the composites. It was observed that the nanoindentation Young's modulus and hardness of the HA/collagen composite materials seem to achieve maximum values for 45-60% HA content by weight. © 2007 Wiley Periodicals, Inc.