Advances in metamaterials and metasurfaces have enabled unprecedented control of light-matter interactions. Metamaterial constituents support high-frequency electric and magnetic dipoles, which can be used as building blocks for new materials capable of negative refraction, electromagnetic cloaking, strong visible-frequency circular dichroism, and enhanced magnetic or chiral transitions in ions and molecules. However, most metamaterials to date have been limited to solid-state, static, narrow-band, and/or small-area structures. Here, we introduce the design, fabrication, and three-dimensional nano-optical characterization of large-area, dynamically-tunable metamaterials and gram-scale metafluids. First, we use transformation optics to design a broadband metamaterial constituent - a metallo-dielectric nanocrescent - characterized by degenerate electric and magnetic dipoles. A periodic array of nanocrescents exhibits large positive and negative refractive indices at optical frequencies, confirmed through simulations of plane wave refraction through a metamaterial prism. Simulations also reveal that the metamaterial optical properties are largely insensitive to the wavelength, orientation and polarization of incident light. Then, we introduce a new tomographic technique, cathodoluminescence (CL) spectroscopic tomography, to probe light-matter interactions in individual nanocrescents with nanometer-scale resolution. Two-dimensional CL maps of the three-dimensional nanostructure are obtained at various orientations, while a filtered back projection is used to reconstruct the CL intensity at each wavelength. The resulting tomograms allow us to locate regions of efficient cathodoluminescence in three dimensions across visible and near-infrared wavelengths, with contributions from material luminescence and radiative decay of electromagnetic eigenmodes. Finally, we demonstrate the fabrication of dynamically tunable large-area metamaterials and gram-scale metafluids, using a combination of colloidal synthesis, protein-directed assembly, self-assembly, etching, and stamping. The electric and magnetic response of the bulk metamaterial and metafluid are directly probed with optical scattering and spectroscopy. Using chemical swelling, these metamaterials exhibit reversible, unity-order refractive index changes that may provide a foundation for new adaptive optical materials in sensing, solar, and display applications.