Inspired by self-assembly of nano-hydroxyapatite (nHA) on collagen associated with the 67nm periodic microstructure of collagen, we used multi-walled carbon nanotubes (MWCNTs) with approximately 40nm bamboo periodic microstructure as a template for nHA deposition to form a nHA-MWCNT composite. The assembled apatite was analyzed by transmission electron microscopy and scanning electron microscopy. Defects that were analogous to edge dislocations along the carbon nanotubes' multi-walled surfaces were the nucleation sites for nHA after these defects had been functionalized principally into carboxylic groups. Spindle-shaped units consisting of an assembly of near parallel, fibril-like nHA polycrystals were formed and oriented at a certain angle to the long axis of the carbon nanotubes, unlike nHA-collagen in which the nHA is oriented along the longitudinal axis of the collagen molecule. One possible explanation for this difference is that there are more bonds for calcium chelation (-COOH, >CO) on the collagen fibril surface than on the surface of MWCNTs. Spindle-shaped units that are detached from the MWCNT template are able to maintain the ordered parallel structure of the nHA polycrystal fibril. We have thus created a self-assembled hydroxyapatite on MWCNTs.