Microcantilever sensor technology has been steadily growing for the last 15 years. While we have gained a great amount of knowledge in rnicrocantilever bending due to surface stress changes, which is a unique property of microcantilever sensors, we are still in the early stages of understanding the fundamental surface chemistries of surface-stress-based microcantilever sensors. In general, increasing surface stress, which is caused by interactions on the microcantilever surfaces, would improve the S/N ratio and subsequently the sensitivity and reliability of microcantilever sensors. In this review, we will summarize (A) the conditions under which a large surface stress can readily be attained and (B) the strategies to increase surface stress in case a large surface stress cannot readily be reached. We will also discuss our perspectives on microcantilever sensors based on surface stress changes.