•CNT network size and interphase in nanomembranes is a crack arrestor mechanism.•Pre-infused BP has a large interphase thickness to network size ratio than a dry BP.•Weibull analysis shows a robust entangled structure of CNTs in pre-infused BP.•Pre-infused BP enhances multimodal fracture toughness in polymer composites.•A robust CNT network/interphase causes crack deflections in BP membranes. Delamination is one of the primary damage mechanisms in laminated composites that affects the lifetime integrity of the composite systems. The present study examines the effects of Buckypaper (BP) nano-reinforcement on the multimodal interlaminar fracture properties of the carbon fiber reinforced polymer (CFRP) composites reinforced with BP membranes. The novelty and the focus of this study is the effects of multi-wall carbon nanotube (MWCNT) network size and interphase in the interlaminar fracture toughness of BP nanocomposites. Dry and pre-infused non-functionalized MWCNT BP were integrated at the mid layer of the composite before laminate curing. The Atomic Force Microscopy Peak Force Quantitative Nanomechanics Mapping (AFM PFQNM) technique and the Weibull model were applied to study the effects of random CNT network size and interphase on mode I, II, and mixed-mode I-II fracture properties. Weibull analysis of 150 dry and pre-infused BP data confirms a high scatter of CNT network size in dry BP compared to pre-infused BP. Weibull modulus of CNT network size (2.33 for large size and 5.18 for small size) and interphase thickness (3.46) show a robust, consistent entangled structure of CNTs in pre-infused BP. Dry BP improves the propagation energy release rate of the CFRP laminates up to 54%. However, it does not provide additional toughening in the initiation crack energy for modes I, II, and I-II. Mode I initiation and propagation, mode II initiation and mixed-mode I/II fracture energy of pre-infused BP nanocomposites are ∼33%, ∼52.5%, ∼14%, and ∼28% higher than the reference. The interlaminar crack either moves exclusively through the BP layer by circumventing the rigid CNT networks or moves forward through the interface of the carbon fiber monofilament above and below the reinforcing BP layer. This saw-like interlaminar crack path triggers numerous toughening mechanisms such as nano-toughened epoxy, nanoscale CNT bridging and pullout, and crack deflection, and it increases the total crack propagation path. Display omitted