Termite mounds are replete with natural nanoparticles, and they vary in physicochemical, geochemical, mineralogical, and biological properties from the adjoining soils. Although termite mounds have wide ecological and environmental roles including soil formation, faunal and vegetation growth and diversity, organic matter decomposition, geochemical exploration, water survey, treatment of underground contamination, thermoregulation, gas exchange, and global climate change, their nanoscale structures made by the associated organomineral complexes are still poorly understood because of technical limitations. In this review, we highlight the ecological and environmental significance of termite mounds and the documented techniques that have been successfully used to study nanostructure of termite mounds, namely, midinfrared spectroscopy (MIRS), photogrammetry and cross-sectional image analysis, a combination of transmission electron microscopy (TEM) and pyrolysis field ionization mass spectrometry (Py-FIMS), scanning transmission X-ray microscopy (STXM) using synchrotron radiation in conjunction with near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, and high-resolution magic angle spinning nuclear magnetic resonance (HR-MAS NMR) for further appraisals. +ere is a need to continually develop and integrate nanotechnology with the routine classical soil analysis methods to improve our understanding of the functional mechanisms of nanostructure of termite mounds that are responsible for specific properties. In view of the numerous roles termite mounds play in the environments, agriculture, and engineering, there is no better time to channel much research into understanding how they function at nanoscale.