This work examines the crack-arresting capability of PEI and PVDF thermoplastic interlayers in short-glass fiber modified and core-shell rubber toughened epoxy materials under mode-I fracture loading. Experimental results show that the initial crack can be effectively arrested by the thermoplastic-epoxy interface and reinitiation of this crack at the thermoplastic layer requires up to 2.5 times higher load than the crack initiation load of the pristine epoxies. The interlayered designs also exhibit a significant increase in energy absorption by up to 43 times more than their pristine counterparts. Competing damage mechanisms and failure events are captured by microscopy images, digital image correlation and high-speed photography observations. Additionally, elasto-plastic fracture mechanics models based on configurational material forces theory are developed for a preliminary crackarresting material selection and to elucidate the material inhomogeneity effects.