Direct Laser Writing (DLW) has been increasingly selected as a microfabrication route for efficient, cost‐effective, high‐resolution material synthesis and conversion. Concurrently, lasers participate in the patterning and assembly of functional geometries in several fields of application, of which electronics stand out. In this review, recent advances and strategies based on DLW for electronics microfabrication are surveyed and outlined, based on laser material growth strategies. First, the main DLW parameters influencing material synthesis and transformation mechanisms are summarized, aimed at selective, tailored writing of conductive and semiconducting materials. Additive and transformative DLW processing mechanisms are discussed, to open space to explore several categories of materials directly synthesized or transformed for electronics microfabrication. These include metallic conductors, metal oxides, transition metal chalcogenides and carbides, laser‐induced graphene, and their mixtures. By accessing a wide range of material types, DLW‐based electronic applications are explored, including processing components, energy harvesting and storage, sensing, and bioelectronics. The expanded capability of lasers to participate in multiple fabrication steps at different implementation levels, from material engineering to device processing, indicates their future applicability to next‐generation electronics, where more accessible, green microfabrication approaches integrate lasers as comprehensive tools.

Since the discovery of laser-induced graphene (LIG), significant advances have been made to obtain green LIG (gLIG) from abundant, eco-friendly, natural, and organic renewable bio-based carbon sources. Recently, some sustainable and cost-effective electronic devices have been designed with gLIG, resulting in diverse solutions to the environmental impact caused by electronic waste (e-waste). However, there are still several challenges that must be addressed regarding the widespread market implementation of gLIG-based products, from synthesis to practical applications. In this review, we focus on sustainable precursor sources, their conversion mechanisms, physical and chemical properties and applications, along with the challenges related to its implementation, showing the future opportunities and perspectives related to this promising new material. Various systems based on gLIG for energy storage, electrocatalysis, water treatment, and sensors have been reported in the literature. Additionally, gLIG has been proposed for ink formulation or incorporation into polymer matrices, to further expand its use to non-carbon-based substrates or applications for which pristine LIG cannot be directly used. In this way, it is possible to apply gLIG on diverse substrates, aiming at emerging wearable and edible electronics. Thus, this review will bring an overview of gLIG developments, in accordance with the European Green Deal, the United Nations Sustainable Development Goals and the new era of internet-of-things, which demands cost-effective electronic components based on the principles of energy efficiency and sustainable production methods.

Laser-induced graphene (LIG) is as a promising material for flexible microsupercapacitors (MSCs) due to its simple and cost-effective processing. However, LIG-MSC research and production has been centered on non-sustainable polymeric substrates, such as polyimide. In this work, it is presented a cost-effective, reproducible, and robust approach for the preparation of LIG structures via a one-step laser direct writing on chromatography paper. The developed strategy relies on soaking the paper in a 0.1 M sodium tetraborate solution (borax) prior to the laser processing. Borax acts as a fire-retardant agent, thus allowing the laser processing of sensitive substrates that other way would be easily destroyed under the high-energy beam. LIG on paper exhibiting low sheet resistance (30 Ω sq⁻¹) and improved electrode/electrolyte interface was obtained by the proposed method. When used as microsupercapacitor electrodes, this laser-induced graphene resulted in specific capacitances of 4.6 mF cm⁻² (0.015 mA cm⁻²). Furthermore, the devices exhibit excellent cycling stability (> 10,000 cycles at 0.5 mA cm⁻²) and good mechanical properties. By connecting the devices in series and parallel, it was also possible to control the voltage and energy delivered by the system. Thus, paper-based LIG-MSC can be used as energy storage devices for flexible, low-cost, and portable electronics. Additionally, due to their flexible design and architecture, they can be easily adapted to other circuits and applications with different power requirements. Graphical Abstract

Laser-induced graphene (LIG) has gained preponderance in recent years, as a very attractive material for the fabrication and patterning of graphitic structures and electrodes, for multiple applications in electronics. Typically, polymeric substrates, such as polyimide, have been used as precursor materials, but other organic, more sustainable, and accessible precursor materials have emerged as viable alternatives, including cellulose substrates. However, these substrates have lacked the conductive and chemical properties achieved by conventional LIG precursor substrates and have not been translated into fully flexible, wearable scenarios. In this work, we expand the conductive properties of paper-based LIG, by boosting the graphitization potential of paper, through the introduction of external aromatic moieties and meticulous control of laser fluence. Colored wax printing over the paper substrates introduces aromatic chemical structures, allowing for the synthesis of LIG chemical structures with sheet resistances as low as 5 Ω·sq^-1, translating to an apparent conductivity as high as 28.2 S·cm^-1. Regarding chemical properties, I_D/I_G ratios of 0.28 showcase low defect densities of LIG chemical structures and improve on previous reports on paper-based LIG, where sheet resistance has been limited to values around 30 Ω·sq^-1, with more defect dense and less crystalline chemical structures. With these improved properties, a simple transfer methodology was developed, based on a water-induced peel-off process that efficiently separates patterned LIG structures from the native paper substrates to conformable, flexible substrates, harnessing the multifunctional capabilities of LIG toward multiple applications in wearable electronics. Proof-of concept electrodes for electrochemical sensors, strain sensors, and in-plane microsupercapacitors were patterned, transferred, and characterized, using paper as a high-value LIG precursor for multiples scenarios in wearable technologies, for improved sustainability and accessibility of such applications.