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Abstract Over the past three decades, nanoindentation has continuously evolved and transformed the field of materials mechanical testing. Once highlighted by the groundbreaking Oliver–Pharr method, the utility of nanoindentation has transcended far beyond modulus and hardness measurements. Today, with increasing challenges in developing advanced energy generation and electronics technologies, we face a growing demand for accelerated materials discovery and efficient assessment of mechanical properties that are coupled with modern machine learning-assisted approaches, most of which require robust experimental validation and verification. To this end, nanoindentation finds its unique strength, owing to its small-volume requirement, of fast-probing and providing a mechanistic understanding of various materials. As such, this technique meets the demand for rapid materials assessment, including semiconductors, ceramics, and thin films, which are integral to next-generation energy-efficient and high-power electronic devices. Here, we highlight modern nanoindentation strategies using novel experimental protocols outlined by the use of nanoindentation for characterizing functional structures, dislocation engineering, high-speed nanoindentation mapping, and accelerating materials discovery via thin-film libraries. We demonstrate that nanoindentation can be a powerful tool for probing the fundamental mechanisms of elasticity, plasticity, and fracture over a wide range of microstructures, offering versatile opportunities for the development and transition of functional materials. Graphical abstract