In recent years, fabrication of inorganic–organic composites mimicking the composite nature of bone has attracted research interest in the field of bone regeneration. Over the last decade, nanosized and nanocrystalline apatite (Ap) has been of special interest to dentistry, the orthopedic industry and nanomedicine because of their excellent performance. ɛ-Polylysine (ɛ-PL) is non-toxic, biodegradable, water soluble natural homopolymer with potential applications in medicine. ɛ-PL is a cationic surface active agent due to its positively charged amino group in water. In last decade experimental work has been done investigating the interactions of various macromolecules of acidic amino acids with hydroxyapatite. In this study, novel bioactive nanostructured composites for bone tissue engineering were developed based on ɛ-PL and apatite (Ap). This composite biomaterial would combine the chemical and biological functionality of ε-PL and bioactivity of Ap.