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One issue of Homogeneous Charge Compression Ignition (HCCI) engines that should be addressed is to suppress rapid combustion in the high-load region. Supercharging the intake air so as to form a leaner mixture is one way of moderating HCCI combustion. However, the specific effect of supercharging on moderating HCCI combustion and the mechanism involved are not fully understood yet. Therefore, experiments were conducted in this study that were designed to moderate rapid combustion in a test HCCI engine by supercharging the air inducted into the cylinder. The engine was operated under high-load levels in a supercharged state in order to make clear the effect of supercharging on expanding the stable operating region in the high-load range. HCCI combustion was investigated under these conditions by making in-cylinder spectroscopic measurements and by analyzing the exhaust gas using Fourier transform infrared (FT-IR) spectroscopy.