The exceptional properties of carbon nanotubes (CNTs) make them ideal nanofillers for various composite materials. In carbon fiber-reinforced polymer (CFRP) composites. CNTs can be grown on the carbon fiber surface to act as a third interface between the fiber and the matrix. However, it was established that the uncontrolled random growth of CNTs could exacerbate delamination in composite structures. Thick nanofiller films could hinder the epoxy from seeping into the carbon fiber, resulting in insufficient interlaminar strength. Hence, the density and distribution of nanofillers play a crucial role in determining the hybrid composite fracture mechanisms. In this investigation, CNTs were grown using the low-temperature technique into specific patterns over carbon fibers to discern their derived composites’ fracture properties. The composite fracture energy release was probed using a double cantilever beam (DCB) test setup and digital image correlation (DIC) to monitor interlaminar crack propagation. A standard finite element simulation model based on the cohesive zone method (CZM) was also utilized to delineate fracture behaviors of the various composite configurations. Results conclude that a coarser pattern of CNT growth enhances resistance to crack propagation, thus improving the interlaminar fracture toughness of a composite structure.