Diverse natural organisms possess stimulus-responsive structures to adapt to the surrounding environment. Inspired by nature, researchers have developed various smart stimulus-responsive structures with adjustable properties and functions to address the demands of ever-changing application environments that are becoming more intricate. Among many fabrication methods for stimulus-responsive structures, femtosecond laser direct writing (FsLDW) has received increasing attention because of its high precision, simplicity, true three-dimensional machining ability, and wide applicability to almost all materials. This paper systematically outlines state-of-the-art research on stimulus-responsive structures prepared by FsLDW. Based on the introduction of femtosecond laser-matter interaction and mainstream FsLDW-based manufacturing strategies, different stimulating factors that can trigger structural responses of prepared intelligent structures, such as magnetic field, light, temperature, pH, and humidity, are emphatically summarized. Various applications of functional structures with stimuli-responsive dynamic behaviors fabricated by FsLDW, as well as the present obstacles and forthcoming development opportunities, are discussed.