AbstractPersonal thermal regulation through passive radiative cooling is an effective strategy to achieve sustainable development. Although recent advances have introduced various cooling textile designs, the extensive use of materials unsuitable for common textiles, alongside coating or compositing technologies, not only compromises the wearability and safety of these textiles but also impacts green sustainability. Herein, it is shown that wool is a promising natural material for transferring mid‐infrared human body radiation, but the high absorption in the solar spectrum prohibits wool from achieving satisfactory daytime radiative cooling. Thus the natural wool impregnates zinc ions into the protein chains to form a zinc‐ion woolen (wool‐Zn) fabric. The wool‐Zn fabric can provide humans with a cooling sensation both indoors and daytime outdoors, showing a temperature reduction of 2 °C on human skin indoors and a reduction of 7 °C on artificial skin under direct sunlight, respectively, when covered by wool‐Zn fabrics compared to when covered with cotton. Moreover, the wool‐Zn fabric shows desirable antibacterial properties and durability against washing and abrasion, while maintaining desirable wearability. As a result, the wool‐Zn fabric shows great potential for commercial application in personal thermoregulation and provides an effective avenue toward sustainable energy and environment.