Ca-based porous and rough bioceramic surfaces were coated on zirconium by micro arc oxidation (MAO). Subsequently, an antibacterial chitosan layer was covered on the MAO-coated zirconium surfaces by dip coating method to develop an antibacterial, bioactive and biocompatible composite biopolymer and bioceramic layer for implant applications. The cubic-ZrO2, meta-stable Ca0.15Zr0.85O1.85, and Ca3(PO4)2 were detected on the MAO surface by powder-XRD. The existence of chitosan on the MAO-coated Zr surfaces was verified by FTIR. The micro-pores and thermal cracks on the bioceramic MAO surface were sealed by chitosan coating, while the MAO surface is porous and rough. All elements such as Zr, O, Ca, P and C were homogenously distributed through both surfaces. Moreover, both surfaces indicated hydrophobic properties. However, the contact angle value of the MAO surface was lower than the one of chitosan-based MAO surface. In vitro bioactivity on both surfaces was investigated by XRD, SEM and EDX analyses at post-immersion in simulated body fluid (SBF) up to 14 days. In vitro bioactivity was significantly enhanced on the chitosan-based MAO surface with respect to the MAO surface. In vitro bacterial adhesions on the chitosan-based MAO surfaces were lower compared to the MAO surfaces for Staphylococcus aureus and Escherichia coli.