have been effectively applied toward the realization of functional surfaces with desired wetting capability. However, most reported approaches are hardly immune from multi-stepped, time-consuming, and rigorously-conditioned processes that have tremendously limited their large-scale and high-reproducible production. [13][14][15][16][17][18] To overcome the above deficiencies, it is necessary to escalate both the material as well as its processing technology. As a newly proposed candidate, graphene and its derivatives are very promising for assembling functional structures and smart devices because of unique 2D crystal structure and exceptional mechanical, electrical, chemical, and thermal properties. [22] For tunable wettability, graphene also have shown strong potentiality ascribed to modifiable surface roughness, porous morphology, and fruitful selection of doping methods. For example, through pH control, [23] light irradiation, [24] charge injection, [25] and solvent treatment, [26] graphene films with different hydrophilic or hydrophobic surfaces have been achieved. Followed by shadow-masking or plasma-etching process, patterned wettability can be tuned. [27,28] However, with complex and uncontrollable process, none of these solutions could have achieved the wetting property with both a wide range of continuous control and a high degree of patterning customization. Accordingly, their large-scale applications have been affected unavoidably.Benefiting from a unique one-step direct laser-scribing process for converting aromatic polymer precursors to graphene, [29] laser-induced graphene (LIG) strategy has exhibited vast superiority over traditional methods in terms of high efficiency, low cost, and scalability for fabricating graphene-based devices, ranging from multifunctional composites, [30] supercapacitors, [31] sensors, [32] heaters, [33] to anti-biofouling interfaces, [34] suggesting strong feasibility to meet the demand of multi-scenario applications. As initial trials, LIG was also applied to modulate its wetting properties by controlling processing atmosphere, [35] by adjusting pulse resolution of laser, [36] or by integrating LIG with hydrophobic Functional surfaces with tunable and patternable wettability have attracted significant research interests because of remarkable advantages in biomedicine, environmental, and energy storage applications. Based on combined defocusing and grafting strategy for processing laser-induced graphene papers (LIGPs) with variable surface roughness (58.18-6.08 µm) and F content (0-25.9%), their wettability can be tuned continuously from superlyophilicity (contact angle CA ≈ 0°) to superlyophobicity (CA > 150°), for various liquids with a wide range of surface tensions from 27.5 to 72.8 mN m −1 . In addition to reaching multiple wetting characteristics including amphiphilic, amphiphobic, and hydrophobic-oleophilic states, three designable processes are further developed for achieving LIGPs with various wetting patterns, including hydrophilic arrays or channels, hydrophobic...
