Natural gas is a major fuel source for many industrial and power-generation applications. The primary constituent of natural gas is methane (CH4), while smaller quantities of higher order hydrocarbons such as ethane (C2H6) and propane (C3H8) can also be present. Detailed understanding of natural gas combustion is important to obtain the highest possible combustion efficiency with minimal environmental impact in devices such as gas turbines and industrial furnaces. For a better understanding the combustion performance of natural gas, several important parameters to study are the flame temperature, heat release zone, flame front evolution, and laminar flame speed as a function of flame equivalence ratio. Spectrally and temporally resolved, high-speed chemiluminescence imaging can provide direct measurements of some of these parameters under controlled laboratory conditions. A series of experiments were performed on premixed methane/ethane-air flames at different equivalence ratios inside a closed flame speed vessel that allows the direct observation of the spherically expanding flame front. The vessel was filled with the mixtures of CH4 and C2H6 along with respective partial pressures of O2 and N2, to obtain the desired equivalence ratios at 1 atm initial pressure. A high-speed camera coupled with an image intensifier system was used to capture the chemiluminescence emitted by the excited hydroxyl (OH*) and methylidyne (CH*) radicals, which are two of the most important species present in the natural gas flames. The calculated laminar flame speeds for an 80/20 methane/ethane blend based on high-speed chemiluminescence images agreed well with the previously conducted Z-type schlieren imaging-based measurements. A high-pressure test, conducted at 5 atm initial pressure, produced wrinkles in the flame and decreased flame propagation rate. In comparison to the spherically expanding laminar flames, subsequent turbulent flame studies showed the sporadic nature of the flame resulting from multiple flame fronts that were evolved discontinuously and independently with the time. This paper documents some of the first results of quantitative spherical flame speed experiments using high-speed chemiluminescence imaging.