Several countries have cities located at elevations above 2000 m. Consequently, the internal combustion engines (ICEs) that operate there do not achieve the desired performance and emissions under these atmospheric conditions. One approach to mitigate these effects and, at the same time, address climate change is the use of biofuel–fossil fuel blends. However, ICEs must operate under a wide range of rpm to meet varying workload demands, raising concerns that these fuel blends may not be fully effective in achieving the desired performance and emission outcomes under such conditions. To address this issue, a series of experimental tests were conducted at low and high rpm of a spark-ignition (SI) ICE fuelled with bioethanol–gasoline blends in the ratios of E10, E15, E20, E40, E60, E85, and E100. The tests were conducted at 2600 m above sea level (masl) under various engine loads. The E20 and E40 blends showed outstanding performance at 2700 rpm, achieving high brake power and low emissions of CO2 and HCs. At 4300 rpm, the E40 blend exhibited great performance because the engine produced high brake power and low emissions of CO and NOx. Based on these results, it can be concluded that bioethanol concentrations of between 20 and 40% in the blend effectively compensate for the reduced atmospheric oxygen at high altitudes, enhancing the combustion process in SI-ICEs.