P.X. Chen, Zikai Li, Yifan Chang, Xinrui Yang, Shuaihua Jiang, Wei Qian, Xun Li, Hao Yuan, Zhe Wang, Zuhao Shi, Daping He
Laser-induced graphene (LIG) technology has streamlined the fabrication of patterned graphene for electronics. However, the laser-induced ultrafast kinetics result in the formation of amorphous structures and high electrical resistivity, limiting its applicability in high-performance devices. Herein, we report a facile strategy of expanding interline spacing in LIG line-to-surface growth for constructing high-crystallinity-riveted surface architectures with significantly enhanced electrical conductivity. This approach enables scalable fabrication of highly conductive LIG (3,290 S m –1 ) under ambient conditions. Compared with doping and defect-healing strategies, this in situ optimization requires no additional reagents or high-temperature treatment and enables single-step patterned fabrication. Crucially, we first identify a heterogeneous structure along the vertical scanning direction in LIG lines, comprising defect-enriched, highly crystallized, and amorphous carbon phases. Combined experimental and theoretical analyses reveal that the structural gradient arises from the laser-pulse-induced Gaussian temperature field and far-from-equilibrium reaction dynamics. On this basis, we design an interline spacing exceeding the laser spot diameter to form high-crystallinity-riveted surface architectures, an interval conventionally considered unsuitable for producing high-quality LIG. The optimized LIG demonstrates substantially enhanced performance in electromagnetic shielding, Joule heating, and strain sensing, highlighting its potential for multifunctional, application-tailored devices.