represent the cornerstone of next-generation electronics. [1][2][3] They are promising for skin electronics, [4][5][6] soft robotics, [7,8] medical implants, [9,10] and human-machine interfaces. [11][12][13][14] Thus far, most stretchable electronics are fabricated by integrating active components including sensors, actuators, transistors, and optoelectronic devices with stretchable interconnections onto soft, stretchable substrates to ensure levels of integration, performance, and reliability comparable to those of waferbased systems. [15][16][17][18] Stretchable conductors are critically important in enabling high-speed data transmission, low power consumption, and superior structural robustness in fully integrated stretchable devices or systems. [19] Creating stretchable mechanical structures from nonstretchable metallic materials, such as in-plane serpentines, out-of-plane wrinkles, and fractal networks have been utilized to eliminate or accommodate strains generated from mechanical deformations without compensating device performances. [20,21] Another facile and low-cost route to achieving reliable conductance against strain is to disperse conductive fillers into an intrinsically stretchable polymer matrix to form percolation networks. [22][23][24][25][26][27] Compared to stretchable conductors fabricated from metallic materials with geometrically defined mechanical structures, this approach offers several prominent advantages, including large-area and scalable fabrication, highdensity device integration, and wide-range strain tolerance. [28,29] In these conductive composites, the conductivity-stretchability relationship depends on the structure of percolation networks formed by the conductive fillers. Generally, the electrical conductivity decreases when the composite conductor is being stretched as macroscale stretching inevitably increases the distance between conductive fillers and thus results in impeded charge transport. [30][31][32] Therefore, maintaining high conductivity under high strain imposes a grand challenge.Central to addressing the conductivity-stretchability dilemma is to effectively regulate microstructures of conductive fillers dispersed inside the polymer matrix. [27,29,[33][34][35][36] Reconstructing conductive pathways via reorganization of conductive fillers during mechanical deformations is a promising methodology to address the trade-off between conductivity and stretchability. However, the mobility of conductive fillers is typically restricted by the long polymer chains in elastomers, and thus Printable and stretchable conductors based on metallic-filler-reinforced polymer composites that can maintain high electrical conductivity at large strains are essential for emerging applications in wearable electronics, soft robotics, and bio-integrated devices. Regulating microstructures of conductive fillers during mechanical deformations is the key to reconstructing the conductive pathway and retaining high electrical conductivity, which has proven to be challenging. Here, it is reported ...