Natural gas is regarded as one of the most potential alternative fuels of engines because of its fruitful storage, good obtainable resources, and high octane value, etc. Compared with port fuel injection (PFI), Gasoline direct injection (GDI) has many advantages on volumetric efficiency improvement, lean-burning, emissions control, etc. A set of measuring and data acquisition system on CNG direct injection spark-ignited engines and the CNG multi-direct injection system are developed in this paper. Based on different injection modes of CNG single DI and compound DI (main injection and auxiliary-Injection), the investigations on combustion process of CNG DI engines has been conducted by the factors of in-cylinder mixture formation, air/fuel ratio, and injection timing, etc. Meanwhile, the three-dimension simulation on mixture formation and combustion principle of low-pressure CNG compound direct injection engines has also been researched. As conclusions, the conception of “Injection window” is issued in this paper, and the theoretic supports and technical measures will be obtained by the testing results and simulation analysis on controlling strategies of the low-pressure CNG direct injection engines.