Disparate natural [9,10] and synthetic [11][12][13][14] constituent materials discoveries, concomitant with the growing diversity of combinatory processing techniques for design of microstructure [15,16] and interphase, [17,18] has expanded both the range and knowledgebase of heterogeneous and composite materials, leading to synergistic mechanical property enhancements in bulk stiffness, strength, and toughness over traditional homogeneous engineering materials, [19][20][21] while often also permitting interdisciplinary strategies for multifunctionality (thermal, electrical, optical, etc.). [22,23] Several cross-cutting research themes have emerged for mechanical property engineering via composite nano-and microstructural heterogeneity and anisotropy, including additive manufacturing, [24][25][26] biomimetics, [27][28][29] and hybrid advanced composites. [30,31] However, incomplete understanding of complex structure-property relationships, [32,33] particularly progressive damage in tough heterogeneous systems built from brittle constituents, has emerged as a unifying theme limiting further performance enhancement among the breadth of cutting-edge advanced materials for structural applications. Fundamental knowledge of heterogeneous material mechanics across scales, particularly as related to "failure," strongly limits performance predictive capabilities as well as rational nano/microstructural design toward optimization. [34][35][36] Motivated by ongoing failure prediction challenges faced globally by academia, government, and industry, aerospace-grade advanced composites exemplify the reality of costly (≈$100M [37] and up to 20 years [38,39] for new materials insertion), experimentally driven qualification campaigns, incurring materials design restrictions and conservative safety margins that undercut theoretical structural efficiency. [40,41] The next advances in mechanical performance understanding are underpinned by higher-fidelity experimental characterizations (especially temporal data) [33] of complex failure processes comprising multiscale, multimodal (multiclass) interacting progressive damage [23,35,36] that inform and validate predictive models for design. Relative to conventional destructive microscale damage characterization techniques [42] like optical and electron microscopy (2D) and acoustic signaling/scanning (low resolution, <3D), synchrotron radiation computed Four-dimensional quantitative characterization of heterogeneous materials using in situ synchrotron radiation computed tomography can reveal 3D sub-micrometer features, particularly damage, evolving under load, leading to improved materials. However, dataset size and complexity increasingly require time-intensive and subjective semi-automatic segmentations. Here, the first deep learning (DL) convolutional neural network (CNN) segmentation of multiclass microscale damage in heterogeneous bulk materials is presented, teaching on advanced aerospace-grade composite damage using ≈65 000 (trained) human-segmented tomograms. The trained CNN mach...