date, a variety of active layers including silver nanowires, [10] conductive polymers, [13] and graphene [14,15] have been used to prepare pressure sensors on elastomer substrates by infilling, [16] lithography, [17] screen, or inject-printing techniques. [18] Nevertheless, these methods are either limited by high-cost and complex technical routes, or involve high temperature and toxic processes, which cannot be truly adapted to green, health-focused wearable devices. [19][20][21][22] Therefore, it remains a daunting challenge to build flexible pressure sensors in a facile, cost-effective, and large-area-capable manner. [23][24][25] In 2014, Tour's group reported that the commercial polyimide (PI, Kapton) film can be directly converted into graphene by CO 2 laser scribing, which has attracted widespread attention. [26] Compared with conventional graphene synthesis methods such as mechanical stripping, chemical vapor deposition and chemical reduction, laser scribing enables large-scale, noncontact, mask-free production in an atmospheric environment. [27,28] The resulting product, known as laser-induced graphene (LIG), shows a 3D porous structure with high specific surface area (≈340 m 2 g −1 ), high thermal stability (>900 °C) and excellent sheet resistance (10 Ω sq −1 ) that can be assembled into different flexible sensors for accurate measurement of hydration, [29] strain, [30] pressure, [14,31] temperature, [32] and other parameters of interest. [33,34] Groundbreaking studies have also found the LIG can be synthesis using multiple pulsed-laser irradiation of carbon precursors including natural materials, [35] food, [36] and even nonpolymer materials. [37,38] However, there are still two challenges to achieve high-quality conversion of LIG. First, natural materials contain more combustible substances, such as proteins, sugars and lignin, than polymers. [39,40] The precursor is first amorphous carbonized and then converted to LIG, which usually requires multiple or defocused laser irradiation and the addition of commercial flame retardants. [41] Second, both from polymers and natural resources, the mechanical properties of LIG are poor while the inherent stiffness cannot meet the inevitable deformation in daily use. [14,42,43] A strategy was developed to remedy this deficiency by transferring the LIG obtained from original platform to elastomers. [5,44] Unfortunately, a significant improvement in flexibility is accompanied by a reduction in electrical properties (sheet resistance down from ≈10 to ≈60 Ω sq −1 ), because Latest advances have witnessed the laser scribing of various active materials from synthetic polymers to natural sources without masks, post-treatment, or toxic substances. However, laser induced graphene (LIG) on renewable precursors usually requires flame-retardant pretreatment and multistep pulsed or defocused irradiation. Laser scribing of silicon carbide (SiC) from polydimethylsiloxane (PDMS) is limited by its high transparency over a broad wavelength range. Here, a structural design strategy ...