A perfusion electrodeposition (P-ELD) system was reported to functionalise additive manufactured Ti6Al4V scaffolds with a calcium phosphate (CaP) coating in a controlled and reproducible manner. The effects and interactions of four main process parameters: current density (I), deposition time (t), flow rate (f) and process temperature (T) on the properties of the CaP coating were investigated. The results showed a direct relation between the parameters and the deposited CaP mass, with a significant effect for t (p = 0.001) and t-f interaction (p = 0.019). Computational fluid dynamic (CFD) analysis showed a relatively low electrolyte velocity within the struts and a high velocity in the open areas within the P-ELD chamber, which were not influenced by a change in f. This is beneficial for promoting a controlled CaP deposition and hydrogen gas removal. Optimisation studies showed a minimum t of 6 hours was needed to obtain complete coating of the scaffold regardless of I used and the thickness increased by increasing I and t. Energy dispersive X-ray (EDAX) and X-ray diffraction (XRD) analysis confirmed the deposition of highly crystalline synthetic carbonated hydroxyapatite under all conditions (Ca/P ratio = 1.41). High cell viability and cell-material interactions were demonstrated by in vitro culture of human periosteum derived cells (hPDCs) on coated scaffolds. This study showed that P-ELD provides a technological tool to functionalise complex scaffold structures with a biocompatible CaP layer that has controlled and reproducible physicochemical properties suitable for bone engineering.