This article presents the development of an experimental methodology based on acoustic emission wave detection for determining delamination onset and propagation in carbon fibre composite materials under quasi-static and fatigue loading. Delamination was investigated in quasi-static interlaminar fracture testing over a wide range of mixed-mode ratios ( G_II/ G_T = 0, 0.3, 0.5 and 1) for unidirectional and woven samples. An acoustic emission wave detection method was developed to detect delamination onset, and the corresponding fracture toughness was computed. Interlaminar fracture toughness was also calculated by beam theory and from finite element analysis with the virtual crack closure technique. The mechanical testing results, acoustic emission monitoring and numerical model’s interlaminar fracture toughness were used to define delamination initiation criteria by drawing two-dimensional envelopes corresponding to G_C = f( G_II/ G_T). The acoustic emission wave detection method showed damage accumulation before observable crack propagation, and its failure envelope corresponded to lower fracture energies than the standard test and modelling methods. Mode I fatigue testing with acoustic emission monitoring was performed on the woven samples for different energy release rate ratios ( G_IMAX/ G_IC = 0.3–0.8). A first series of samples were tested to construct an onset delamination fatigue curve Δ G = f( N). A second series of samples were used to study the cumulative acoustic emission energy distribution during delamination growth. An unsupervised pattern recognition methodology is presented for crack opening and closing testing, in order to discriminate between fatigue signal noise and acoustic emission signals emitted from crack initiation and crack growth. Correlations were observed between the acoustic emission energy distribution, the load range, the delamination length and the crack growth rate.