Fuel injection parameters and fuel reactivity significantly affect engine performance, combustion, and emissions. The dual direct-injection strategy could compensate for the insufficient heat release rate to improve the gasoline compression ignition (GCI) mode with medium injection pressure for high loads. This research aims to couple injection parameters and fuel reactivity to optimize the combustion, emissions, and engine performance of the dual direct-injection GCI mode at high loads. The effect of research octane number (RON) of gasoline, injection timing, and injection pressure of dual injection system on combustion and emissions was investigated. Results show that the optimized dual direct-injection GCI mode can simultaneously achieve high thermal efficiency, low emissions, and low maximum pressure rise rate (MPRR) at high loads with the maximum indicated mean effective pressure (IMEP) of about 16 bar with indicated thermal efficiency (ITE) of 48.5%. Delaying the injection timing of injector-1 reduced the peak pressure (Ppeak), MPRR, and NOx emissions. Ppeak, CO, NOx, and indicated specific fuel consumption (ISFC) decreased compared to the dual-injector simultaneous injection case when the injection timing of injector-2 was retarded to between 5 and 10°CA ATDC. Increasing the injection pressure of injector-2 reduced CO, THC, ISFC, and particulate emissions. Lower RON gasoline obtains higher ITE while higher RON gasoline obtains lower particulate emissions.