Chemical-looping combustion offers a promising carbon capture technology for coal-fired power generation. Enhancing the operational flexibility and energy efficiency of such plants is crucial for achieving primary energy savings and renewable energy accommodation. In this study, the operating characteristics of an integrated gasification chemical-looping combustion combined cycle (IGCLCCC) under various loads are studied, and the deterioration mechanism of its thermodynamic performance is revealed. Further, an IGCLCCC scheme coupled with molten salt heat storage is proposed and evaluated from thermodynamic performance and operational flexibility. Study results indicate that the net efficiency of the IGCLCCC reaches 37.7% under 30% load, which is superior to those of conventional CO2 capture power plants under full load. Adopting the heat storage system significantly improves the operational flexibility and energy efficiency of the IGCLCCC by expanding its operating range from 30.0∼100.0% to 25.7∼105.3%. The equivalent round-trip efficiency of the heat storage system reaches 134.6% due to the upgrading of the thermal energy from the exhaust gas of the air turbine from original low levels to high levels driven by the exergy saving during the oxygen carrier-air reaction because of the air preheating to a high temperature.