Volatile organic compounds (VOCs) are a class of organic compounds with high vapor pressure and low boiling points, widely present in both natural environments and human activities. VOCs released from various sources not only contribute to environmental pollution but also pose threats to ecosystems and human health. Moreover, some VOCs are considered biomarkers in exhaled breath and can be utilized to identify various diseases. Therefore, monitoring and controlling VOC emissions and concentrations are crucial for safeguarding the environment and human health. In recent years, significant advancements have been achieved in micro‐electromechanical system (MEMS)‐based sensing and optical sensing technologies, offering new avenues for VOC detection. This article provides a comprehensive overview of research progress in MEMS and optical VOC sensors, focusing on their sensing mechanisms and classifications. It then discusses the role of artificial intelligence in enhancing VOC identification and quantification, as well as trends toward sensor miniaturization and intelligence. Furthermore, the article highlights the diverse applications of VOC sensors in medical diagnostics, agricultural food testing, and the Internet of Things. Finally, it emphasizes the opportunities and challenges associated with MEMS and optical VOC sensors, providing valuable insights for practical applications.