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Structures can develop damage throughout their operational lifetimes, typically due to excessive loading, harsh environmental and loading conditions, and long-term deterioration. To evaluate the condition of structures, conventional structural health monitoring (SHM) systems employ discrete sensors such as accelerometers, displacement transducers, and strain gages, among others. Although these sensors provide quantitative data that can be correlated to structural behavior, it remains challenging to accurately detect and locate damage effectively. This chapter presents a summary of recent developments in using carbon nanotubes for the design of nanocomposite thin films that are sensitive to damage (specifically strain). In particular, the chapter presents in great detail the design and strain-sensing properties of three different types of nanofilms: buckypaper, layer-by-layer, and spray-coated films. In addition …