Recent advances and demands in clinical applications drive a large amount of research to hydroxyapatite (HA) composite coatings fabricated by plasma spray. However, lower degree of HA crystallinity related to high temperature exposure in plasma spray usually leads to rapid weakening and disintegration of HA coatings and often promotes inflammatory responses in the surrounding tissue. In this research, graphene nanosheet (GNS) reinforced HA coatings were fabricated using plasma spray and followed by heat and hydrothermal treatment (hereafter referred to as thermal treatment). The addition of GNSs resulted in competing phenomenon to influence HA crystallinity viz. increased portion of the partially melted/unmelted zones and higher cooling rate during splat formation, leading to slight increase in HA crystallinity (~46.0-51.3%) in the as-sprayed coating. XRD and FTIR results showed that thermal treatment was capable of inducing significant transformation of amorphous HA to the crystalline form and removing other foreign non-HA compounds through regaining OH- ion, and therefore HA coatings displayed ~45.5-47.1% improvements in HA crystallinity regardless of addition or not of the GNS nanofillers. Microstructure observations revealed that thermal treatment enabled microcrack propagation due to stresses caused by crystallisation and phase transformations, and the residual partially melted/unmelted zone of the thermally treated GNS/HA coating was significantly decreased in size. More importantly, the added GNSs contributed greatly to the significant increase in surface nanoroughness of the thermally treated HA coatings owing to the fact that much more structural defects along with the GNSs mainly induced by thermal treatment might act as nucleation sites to accelerate HA nanoparticle precipitation, which would be beneficial for the improved adhesion strength of the osteoblast cells on the coating surface.