The prominent aim of this investigation was the examination of the in-principle feasibility of aluminum combustion under internal combustion engine (ICE)-like conditions. This study was performed in the framework of recent consideration of metallic nanoparticles as alternative fuels for ICE engines. Aluminum nanoparticles of different morphologies and sizes were studied with respect to their fundamental oxidation characteristics via thermogravimetric analysis under various nitrogen oxygen environments and by spark-ignition of Al nanopowder "strips" under controlled airflow at ambient pressure. The ICE-like tests included measurements performed in two different arrangements; namely, a shock-tube setup and a constant-volume combustion vessel. A set of engine tests was also performed in a single-cylinder compression-ignition engine with a customized, single-shot aerosol injection system. Burned powder samples were, in all cases, examined via in situ and ex situ techniques for the identification of products and their morphologies. The results largely verified that combustion of aluminum particles in an engine environment is indeed feasible. Nonetheless, prominent differences, in terms of the products formed and their morphologies/structures, were identified among the various oxidation/combustion techniques employed.