Developing fracture-resistant high-strength steels is an attractive prospect for various structural applications. In this work, a combination of carburizing heat treatment (CHT) and shot peening (SP) was used to develop combined strengthening (CS) mechanisms and to improve the mechanical strength and dynamic fracture toughness of 18CrNiMo7-6 alloy steel. Standard tensile tests and split Hopkinson pressure bar tests were conducted to investigate the strength and dynamic fracture toughness of the 18CrNiMo7-6 alloy steel. The crack initiation and propagation of samples were studied using scanning electron microscopy and transmission electron microscopy. Microstructure characterization and molecular dynamic simulations indicated that the excellent dynamic fracture toughness of the CS samples could be attributed to the grain refinement after strengthening and the formation of numerous slip bands at the crack tips, reducing the stress concentration at the crack tips. The Cr23C6 precipitates have a positive effect on the strength improvement of 18CrNiMo7-6 alloy steel. The results showed that this research can be used to guide the design of steels with high-strength and high-dynamic fracture toughness.