There is growing international interest in hard biocompatible thin film surface coatings to extend the lifetime of medical implants. Parameters of the physical vapour deposition technique can be utilized to fine tune the microstructure and resulting properties of the growing thin film surface by modifying the adatom mobility of the incoming species. This work investigates the evolution of high hardness and biocompatibility of sputter deposited beta-Ti3Au intermetallic thin film surfaces as a function of growth temperature and pressure. Titanium and gold are sputtered in an optimised 3:1 ratio over glass and Ti6Al4V substrates at varying pressures of 0.3 to 1.2 Pa and temperatures of 25 to 450°C. The microstructure and crystallinity of the deposited films improved with reduction in pressure from 1.2 to 0.3 Pa but development of the β-Ti3Au intermetallic compound occurred at temperatures above 350˚C. The density of the films also increased with reducing pressure, whereas improvement in their columnar structure was observed with increasing substrate temperature. These microstructural changes caused by adatom mobility variation, led to the emergence of superior mechanical surface hardness, reaching a peak value of 12.5 GPa for films grown at 0.3 Pa and 450°C. All thin film surfaces were highly biocompatible with ion leaching levels below 1 ppm, and films deposited at lower pressure exhibited much safer cytotoxic profiles against L929 mouse fibroblasts. This work demonstrates the emergence of high hardness and biocompatibility in Ti3Au thin film surfaces with potential as next generation medical implant coating materials.