Organic-inorganic composites composed of organic polymer and carbonate hydroxyapatite (CHAp) would be useful bone substitute materials exhibiting low young’s modulus and bone-bonding bioactivity. In this work, such a composite was synthesized from cellulose (CEL)and CHAp through mechanochemical reaction. Homogeneous bulk CEL-CHAp composites were obtained when poly( ε-caprolactone) (PCL) was added as plasticizer with PCL/(PCL+CEL) weight ratio of 20 wt% or less. The CEL-CHAp composites contained B-type CHAp in inorganic phase. The composites with (CEL+PCL)/(CHAp) weight ratio = 20/80 and 10/90 kept the shape in simulated body fluid (SBF), and showed apatite formation after soaking in SBF. Therefore, the CEL-CHAp composites are expected to be materials with low young’s modulus and bioactivity.