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To explore the exergy loss of engine combustion process, entropy generations were numerically analyzed through detailed chemical kinetics. It revealed that the reformed fuel with simpler molecular tended to produce lower combustion irreversibility. Furthermore, a promising high efficiency RM- HCCI (Reformed molecule HCCI) combustion principle was proposed. In a RM-HCCI engine, hydrocarbon fuels were reformed into small molecule fuels under high temperature and low/no oxygen atmosphere before injection into the cylinder when the exhaust gas enthalpy to a certain extent was recovered, further improving the engine efficiency. The second law efficiency (η2nd) of a RM-HCCI combustion with a CR of 10 can be increased from 36.78% to 45.47% by coordination of multiple control parameters, and to 67.79% by raising CR from 10 to 100.