In recent years there has been an increased interest in raising the octane level of gasoline to enable higher compression ratios (CR) in spark-ignition engines to improve vehicle fuel efficiency. A number of studies have examined opportunities to increase efficiency in future vehicles, but potential impacts on the legacy fleet have not received as much attention. This effort focused on experimental studies on an engine using high-octane fuels without changing the engine’s CR. Spark timing was advanced until maximum torque was reached or knock was encountered for each engine condition, using each individual fuel to maximize engine efficiency. Knock-limited conditions occurred as the output brake mean effective pressure (BMEP) neared the maximum attainable output at a given engine speed. Increasing research octane numbers generally enabled knock-free operation under a greater number of operating conditions. Vehicle modeling using Autonomie was used to project vehicle energy use, fuel economy, and tailpipe CO2 emissions for the Urban Dynamometer Driving Schedule (UDDS), the Highway Fuel Economy Test (HWFET), and the US06 cycle. Results show that decreases in energy consumption of up to 2% for a small SUV are possible through the use of a 97 RON fuel compared to a baseline using 91 RON fuel, provided that the formulation of the fuel does not cause unanticipated operational issues such as lower maximum BMEP. Greater improvements using high-octane fuels are possible if the CR is increased, but there is no opportunity to increase the CR in legacy vehicles. Thus, these vehicles realize an improvement from increased octane rating in accordance with their ability to spark advance to take advantage of a fuel with a higher octane rating. For the modeled vehicle, improvements of up to 2% in volumetric fuel economy may be possible through the use of a 97 RON fuel with the largest gains expected on the US06 cycle. Fuel economy impacts are strongly coupled to the heating value of the fuels in addition to changes in engine efficiency. Similarly, decreases in tailpipe CO2 emissions are also achievable. However, simultaneous improvements in energy consumption, fuel economy, and tailpipe CO2 emissions are not guaranteed and are dependent upon fuel formulation.