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 ?ber-based multimodal sensors simultaneously

remains a great challenge. Here, a smart ?ber 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 ?ber

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 e?ciency 72.9%). Unlike

traditional ?ber-based sensors where elaborate nanostructures are prone to

shedding during knitting, this strategy enables the ?ber sensors with excellent

knittability to be patterned in the fabric, improving both optical and electrical

sensitivities. This work is anticipated to make a signi?cant contribution to the

further development of wearable electronic products and visual

human–computer interaction electronic devices.