Grain-oriented calcium hydroxyapatite (HA) ceramics are potential to enhance or select their bioactive properties. In the current work, highly a-axis oriented calcium HA bulk and thick film samples were prepared by a novel process combining magnetic alignment and polymerization techniques. The slurry containing 40 vol.% commercial HA powder, monomer, initiator and catalyst were poured into a rubber mold for bulk samples or drop-coated on Al 2 O 3 substrate for films at first, and then moved them into a vertical 10 T magnetic field. The HA particles in the low viscosity slurry were aligned by magnetic force and then in situ locked via polymerization of the slurry. After sintering, the grain-oriented HA ceramic bulk and thick film samples with a-axis parallel to the magnetic field direction were obtained. Theoretically, the grain-orientation can be easily controlled by adjusting the magnetic field direction.