Internal combustion engines (ICEs) are essential for the welfare of today’s human civilization yet they contribute to almost 10% of the global CO2 emissions. Reducing the carbon footprint of the ICEs can be achieved by either increasing the engine efficiency to reduce fuel consumption or the utilization of carbon-neutral fuels. This dissertation aims to investigate the effect of the oxidizer composition on the efficiency and performance of the homogenous charge compression ignition (HCCI) engine. It also aims to study the behavior of hydrogen in HCCI engines. The experiments are conducted using a Cooperative Fuel Research (CFR) engine. The study also involves using chemical kinetics simulations to estimate the ignition delay time of hydrogen which is relevant to the HCCI mode of combustion. The results suggest that the specific heat ratio of the oxidizer does not significantly affect the HCCI engine efficiency. On the fuel side, hydrogen showed high sensitivity to engine running conditions due to the lack of negative temperature coefficient (NTC).