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Natural gas (NG) engines have very broad application prospects. The pilot-ignited NG diesel engine can be organized into two combustion modes according to the sequence of oil and gas injection: (1) High-pressure direct injection, where NG is mainly diffused combustion; and (2) partially premixed compression ignition, where NG is mainly premixed combustion. In this study, we used CONVERGE to explore the influence of the NG injection timing on the distribution of the mixture equivalence ratio, ignition characteristics, thermal efficiency, emission, and combustion reaction rate under the two combustion modes. We also used a multi-step soot model to analyze the particle mass and quantity. We showed herein that the NG injection timing significantly affects the mixture distribution in the cylinder, thereby consequently affecting the combustion process. Both very early and very late injection times were not conducive to NG combustion. In addition, the mass, quantity, and diameter of the soot produced by diffusion combustion were larger than those produced with premixed combustion. [ABSTRACT FROM AUTHOR]