With the depletion of hydrocarbon fuels, the hydrogen-hydrocarbon combustion system provides a good solution for the transition period from a hydrocarbon-based energy sys- tem to a hydrogen-based energy system because of its desirable combustion characteristics and the low level of modification to current combustion systems. Though extensive re- search has been carried out to investigate the combustion process of hydrogen-hydrocarbon fuels, no experiments have been reported to study the Particulate Matter (PM) formations in hydrogen-hydrocarbon combustion systems. To measure the PM concentrations in a laminar diffusion flame, a new optical diagnostic technique, called Cone-Beam Tomographic Three Colour Spectrometry (CBT-TCS) has been developed to measure the spatially distributed temperature, soot diameter and soot volume fraction. This technique is based on the principle of three colour pyrometry, but uses a more rigorous light scattering model to calculate the soot diameter and soot volume fraction. The cone beam tomography technique has also been used to reconstruct the 3D property fields from the 2D flame images. The detailed theoretical principles, the exper- imental setup, the optical considerations, the reconstruction algorithm and the sensitivity analysis are all introduced. The CBT-TCS technique has been successfully applied to several laminar diffusion flames to study the PM formation. The temperature and soot volume fracction profiles measured by CBT-TCS for a ethylene laminar diffusion flame are consistent with the data reported by Snelling et al. [77]. The helium-ethylene-air flame tests show that adding helium reduces the PM formation (due to the dilution effect). The hydrogen-ethylene-air flame tests show that adding hydrogen is more effective in reducing the PM formation due to the combined effect of dilution and direct chemical reaction. A PM sampling system has also been de- veloped to verify the PM size distributions measured by CBT-TCS. The comparison results show that the CBT-TCS tends to overestimate the particle size. Several optical engine experiments have also been undertaken to investigate the effect of adding hydrogen on the PM emissions from a Gasoline Direct Injection (GDI) engine. The hydrogen-ethylene engine tests show that adding hydrogen can reduce the PM emissions without sacrificing the power output. The hydrogen-base fuel (65% isooctane and 35% toluene) tests show that adding hydrogen can improve the combustion stability and reduce the PM emissions, especially at low load. Adding 5% stoichiometric of hydrogen can reduce the total PM number concentration by 90% for a stoichiometric mixture and 97% for richer mixture at low load. At high load, adding 10% stoichiometric of hydrogen can also reduce the total PM number concentration by 85% for richer mixture but has little effect upon the stoichiometric mixture.