Four-dimensional time-resolved Synchrotron Radiation Computed Tomography (SRCT) has been used to capture Mode I delamination propagation in particle-toughened Carbon Fibre Reinforced Polymers (CFRPs). Digital Volume Correlation (DVC) was used in order to measure ply opening displacements at the crack tip, permitting the interlayer strain ahead of the crack tip to be quantified. Estimates at which toughening particles de-bonded and/or fractured were made, giving insight into the effects of particle type and particle size on the fracture mico-mechanisms. The experiments are complemented by a 2D plane-strain finite element (FE) model, which investigated the effects of particle strength and toughness on the ply opening displacement and crack path by modelling the particles as 1D cohesive segments. Previous work has shown that Mode I crack propagation in particle-toughened interlayers involves a process zone rather than a distinct crack tip. Therefore, Augmented Finite Element Method (A-FEM) elements were used in the simulation, since the elements can account for both bifurcating and merging cracks within a single element. The nodal displacements in the simulation were compared to the DVC results, illustrating a potential path through which more complex FE simulations may be validated against experimental results in the future.