To determine the effects of buoyancy on the spherical flame and explosion pressure under dilution conditions, a series of explosion experiments were conducted in a 20-L spherical container. The schlieren technique was used to record CH4 flames to assess the buoyancy effect. The change in the explosion pressure was recorded and correlated with the flame shape to analyze the explosion characteristics. The methane explosion occurred in two stages: initial ignition and flame development. During initial ignition, the addition of CO2 caused the flame buoyancy to increase considerably. Flames with different buoyancies had different shapes, such as spherical, ellipsoidal, and “ω” shapes. The radius of the flame at 12 mm may serve as the threshold for the onset of buoyancy effects; once the radius exceeds this value, the flame could deform due to buoyancy effects. Increasing the added CO2 concentration caused the buoyancy effect to be enhanced and appear at a very low radius of the flame. The combined effects of buoyancy and dilution reduced the flame expansion speed. The difference between the horizontal and upward expansion speeds linearly increased with the CO2 concentration. At a high CO2 concentration, the flame stagnated at speeds below 0.5 m/s. During flame development, CO2 addition made the flame surface smoother. Suppressing the cellular flame structure delayed the maximum explosion pressure rise rate and reduced the pressure peak. A coupled analysis of the flame shape and the maximum explosion pressure rise rate showed a dense cellular structure for a high explosion pressure rise rate and a smooth flame surface for a low maximum explosion pressure rise rate. The size and number of cellular structures for different mixtures were similar at a fixed maximum explosion pressure rise rate.