High catalytic activities of enzymes are necessary for enzyme immobilising technology for the development of glucose sensors. The aim of this study is to synthesise two types of poly(L-lysine)-containing calcium phosphate particles (pLys-HAp) and to achieve the immobilisation of glucose oxidase (GOX) on them. The oxidation activity of GOX immobilised on these particles was more than 80% compared to that of native GOX (considered to be 100%). Additionally, the relative activity of GOX immobilised on poly-ε-lysine-containing HAp (ε-pLys-HAp) remained approximately 70% after ten cycles. Moreover, glucose detection was able to be performed in the linear range of 4–400 μM using GOX immobilised on pLys-HAp composites. In the direct electrochemistry measurement using the cyclic voltammetry (CV) method, a glassy carbon electrode (GCE) modified by ε-pLys-HAp was a good enzyme electrode and can be used for glucose detection with high sensitivity. From these results, poly(L-lysine)-containing HAp composites can be expected to be enzyme immobilisation agents with high stability and biosensors with high sensitivity.