Multimodal Scanning Probe Microscopy for Advanced Surface and Interface Characterization

Scanning probe microscopy (SPM) has evolved into a versatile platform for nanoscale characterization with atomic‐scale resolution. Recent advances in multimodal and intelligent SPM have extended conventional imaging by integrating complementary measurements, automated acquisition, artificial intelligence (AI), and machine learning–based analysis. These developments enable direct correlations between nanoscale structures and functional responses in complex interfaces, low‐dimensional materials, quantum systems, energy materials, and biological architectures. This review summarizes the principles, technological advances, and applications of multimodal SPM, including electrical characterization, nanospectroscopy, correlative structure–property mapping, autonomous microscopy, and quantum sensing. Representative applications in nanoelectronics, energy conversion, catalysis, quantum technologies, and functional materials highlight the potential of these approaches for revealing nanoscale phenomena. Finally, challenges and future opportunities, including multifunctional probes, AI‐driven autonomous experimentation, quantum‐enhanced sensing, and high‐throughput description, are discussed. The integration of advanced instrumentation, multimodal data fusion, and intelligent analysis is expected to establish SPM as a next‐generation framework for quantitative surface and interface characterization and accelerated materials discovery.