Uncovering the mechanisms of biomaterial-bone attachment is complicated by the complex and three-dimensional hierarchical structure of human bone. Our work explores the structure and formation of bone and its attachment to biomaterials with advanced microscopy approaches. This talk will introduce a range of correlative, 3D, and real-time high-resolution approaches to probe both biomineralization and osseointegration including electron tomography, focused ion beam microscopy, in situ liquid phase TEM, and atom probe tomography. These correlative microscopies provide a foundation for understanding the structure and chemical nature of inorganic and organic biomaterials, including shedding light on the titanium-bone interface, collagen-mineral arrangement, new approaches for visualizing osteocyte networks, and mineralization events in liquids. These platforms for characterization have broad applications across the field of biomedical engineering.