In order to obtain a higher pressure capacity for the high-pressure die with a larger sample cavity, two types of two-layer split dies with a round cylinder and a quadrate cylinder were designed based on the conventional belt-type die. Finite element analysis was performed to investigate the stress distributions and pressure capacities of the high-pressure dies using a derived Mohr–Coulomb criterion and the von Mises criterion for the cylinder and supporting rings, respectively. As predicted by the finite element analysis results, in the two-layer split dies with a round cylinder, the stress state of the cylinder can be only slightly improved; and the von Mises stress of the first layer supporting ring can be hardly decreased. However, in the two-layer split dies with a quadrate cylinder and sample cavity, the stress state of the cylinder can be remarkably improved. Simultaneously, the von Mises stress of the supporting rings, especially for the first-layer supporting ring, can be also effectively decreased. The pressure capacities of the two-layer split dies with a round cylinder and a quadrate cylinder are 16.5% and 63.9% higher with respect to the conventional belt-type die.