Low thermal efficiency and high hydrocarbon emissions caused by slow combustion rates and high methane emissions hinder the development of natural gas (NG) engines. Engine structure modifications have always been an important means of improving the combustion effects of engines. This study investigates the effects of combustion chamber improvements on the thermal efficiency and hydrocarbon emissions of stoichiometric spark-ignition NG engines through numerical simulations. The improvements aimed to enhance squish flow, organize high tumble flow, and reduce crevice volume. The results indicate that strengthening the squish intensity by increasing the squish area of the piston can accelerate flame propagation and reduce exhaust loss. However, this improvement is hindered by a significant rise in heat transfer loss, which limits further gains in thermal efficiency. Compared to the traditional high swirl combustion chamber, a high tumble combustion chamber (dual straight intake port combined with a hemispherical piston) can promote flame propagation in the early stages of combustion and increase thermal efficiency by 1.43%. However, the accelerated flame propagation rate resulting from increased flow intensity has little potential to reduce hydrocarbon emissions due to the small contribution of flame quenching to unburned hydrocarbon production. The primary source of hydrocarbon emissions from NG engines is unburned methane in the piston crevice. Therefore, when addressing hydrocarbon emissions from NG engines, the first consideration should be to minimize the volume of the piston crevice, which will significantly reduce methane emissions and incomplete combustion loss.