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Fiber‐based multimodal sensors with electrical/optical signals are highly desired for next‐generation wearable electronics. Despite the remarkable progress in this area, achieving large‐scale knittable, washable, and self‐healing performance in fiber‐based multimodal sensors simultaneously remains a great challenge. Here, a smart fiber capable of exhibiting piezoresistive/luminescent properties based on an H‐bonding connected multilayered core–shell nanostructure is developed. The core principle of this design involves constructing strong interfacial interactions between the fiber layers, which results in a sensor with high sensitivity (gauge factor = 12383500), exceptional water resistance, and robust self‐healing properties (tensile strength 30.9 MPa, healing efficiency 72.9%). Unlike traditional fiber‐based sensors where elaborate nanostructures are prone to shedding during knitting, this strategy enables the fiber sensors with excellent knittability to be patterned in the fabric, improving both optical and electrical sensitivities. This work is anticipated to make a significant contribution to the further development of wearable electronic products and visual human–computer interaction electronic devices. [ABSTRACT FROM AUTHOR]