Laser pulses of few a nanoseconds’ duration are focused by an appropriate converging lens system, leading to breakdown of the medium (combustible gases), resulting in the formation of intense plasma. Plasma thus induced can be used to initiate the combustion of combustible air-fuel mixtures in a spark ignition engine provided the energy of the plasma spark is high enough. Laser ignition has several advantages over the conventional spark ignition system, especially in case of lean air-fuel mixture. In this study, laser ignition of compressed natural gas was investigated in a constant volume combustion chamber (CVCC) as well as in a single-cylinder engine. Flame kernel visualizations for different pulse energy of natural gas-air mixtures were carried out in the CVCC. The images of the development of early flame kernel stages and its growth with time were recorded by shadowgraphy technique. The effect of laser pulse energy on the engine combustion, performance, and emissions was investigated using different air-fuel mixtures. Increased peak cylinder pressure, higher rate of heat release, faster combustion, and increased combustion stability were observed for higher laser pulse energies. The effect of laser pulse energy on the engine-out emissions was also investigated in this study.