In the present work, the surface tension and density of a set of Al-Ni alloys have been investigated as a function of composition and temperature. The measurements were performed by the large drop method, under equilibrium and with an oxygen-free surrounding atmosphere to prevent oxidation phenomena. The study was focused mainly on Al-rich alloys investigated in the framework of the EU FP7-IMPRESS project aimed to obtain tailor-made Al-Ni nanopowders for high-performance macroscale catalytic devices. The measured thermophysical properties were compared with both literature results and data theoretically predicted by applying thermodynamic calculation methods (e.g.. QCA and CFM), with the aim to highlight the role of Al-Ni intermetallic compounds.