A dual-fuel approach to control combustion in HCCI engine is investigated in this work. This approach involves controlling the combustion heat release rate by adjusting fuel reactivity according to the conditions inside the cylinder. Experiments were performed on a single-cylinder research engine fueled with different ratios of primary reference fuels and operated at different speed and load conditions, and results from these experiments showed a clear potential for the approach to expand the HCCI engine operation window. Such potential is further demonstrated dynamically using an optimized stochastic reactor model integrated within a MATLAB code that simulates HCCI multi-cycle operation and closed-loop control of fuel ratio. The model, which utilizes a reduced PRF mechanism, was optimized using a multi-objective genetic algorithm and then compared to a wide range of engine data. The optimization objectives, selected based on relevance to this control study, were the cylinder pressure history, pressure rise rate, and gross indicated mean effective pressure (IMEPg). The closed-loop control of fuel ratio employed in this study is based on a search algorithm, where the objective is to maximize the gross work rather than directly controlling the combustion phasing to match preset values. This control strategy proved effective in controlling pressure rise rate and combustion phasing while not needing any prior knowledge or preset information about them. It also ensured that the engine was always delivering maximum work at each operation condition. This is in a sense analogous to the use of maximum brake torque timing in spark-ignition engines. The dynamic model allowed for convenient examination of the dual-fuel approach beyond the limits tested in the experiments, and thus helped in performing an overall assessment of the approach's potential and limitations.