In recent years, there has been an increasing interest in the novel bioinspired sensors, especially for their selectivity, response time, and sensitivity. Particular attention is paid to the novel optical functional materials that are crucial for the sensors to achieve various energy transduction. Ideally, many critical parameters of the optical sensing materials can be appropriately tailored to meet various specific requirements using optimal design. Over a long and cruel evolution, nature's creatures have created a variety of photonic structures. One impressive example is the iridescent wings of butterfly. The natural photonic crystals on its surfaces have inspired diverse novel designs of optical functional sensing materials, especially in the past three years. Herein, this review mainly discusses recent advances of the burgeoning butterfly‐inspired sensing materials with optical properties that can be modulated in response to different external stimuli. First, their optical sensing performance to infrared radiation/thermal, vapor, liquid, pH, and so on are discussed in details. Then, the fabrication methods and their working mechanisms are also introduced. Furthermore, the general strategies of these emerging sensing materials and their potential applications are also discussed in‐depth as well as their limitations and the future challenges.