Graphene has recently been attracting considerable interest because of its exceptional conductivity, mechanical strength, thermal stability, etc. Graphene-based devices exhibit high potential for applications in electronics, optoelectronics, and energy harvesting. In this paper, we review various growth strategies including metal-catalyzed transfer-free growth and direct-growth of graphene on flexible and rigid insulating substrates which are "major issues" for avoiding the complicated transfer processes that cause graphene defects, residues, tears and performance degradation in graphene-based functional devices. Recent advances in practical applications based on "direct-grown graphene" are discussed. Finally, several important directions, challenges and perspectives in the commercialization of 'direct growth of graphene' are also discussed and addressed.

Despite the enormous potential of the single-crystalline two-dimensional (2D) materials for a wide range of future innovations and applications, 2D single-crystals are still suffering in industrialization due to the lack of efficient large-area production methods. In this work, we introduce a general approach for the scalable growth of single-crystalline graphene, which is a representative 2D material, through “transplanting” uniaxially aligned graphene “seedlings” onto a larger-area catalytic growth substrate. By inducing homoepitaxial growth of graphene from the edges of the seeds arrays without additional nucleations, we obtained single-crystalline graphene with an area four times larger than the mother graphene seed substrate. Moreover, the defect-healing process eliminated the inherent defects of seeds, ensuring the reliability and crystallinity of the single-crystalline graphene for industrialization.

Since the first development of large‐area graphene synthesis by the chemical vapor deposition (CVD) method in 2009, CVD‐graphene has been considered to be a key material in the future electronics, energy, and display industries, which require transparent, flexible, and stretchable characteristics. Although many graphene‐based prototype applications have been demonstrated, several important issues must be addressed in order for them to be compatible with current complementary metal‐oxide‐semiconductor (CMOS)‐based manufacturing processes. In particular, metal contamination and mechanical damage, caused by the metal catalyst for graphene growth, are known to cause severe and irreversible deterioration in the performance of devices. The most effective way to solve the problems is to grow the graphene directly on the semiconductor substrate. Herein, recent advances in the direct growth of graphene on group‐IV semiconductors are reviewed, focusing mainly on the growth mechanism and initial growth behavior when graphene is synthesized on Si and Ge. Furthermore, recent progress in the device applications of graphene with Si and Ge are presented. Finally, perspectives for future research in graphene with a semiconductor are discussed.

Graphene, an ultrathin flexible material with high carrier mobility and transparency, is a promising candidate for flexible transparent conducting electrodes (TCEs). However, its resistance is too high for use as a TCE material by itself. Therefore, fabricating graphene with low sheet resistance and high stability is a significant challenge for practical applications of graphene TCEs. In this study, a 2D doping layer (DL) is proposed, which can stably dope graphene to develop a highly transparent graphene TCE with low sheet resistance. For this purpose, the 2D DL is prepared by immobilizing dopant molecules on transparent graphene oxide and simply stacking it with graphene enables efficient and stable charge transfer doping of the graphene. A TCE fabricated by alternately stacking the DL and graphene has a high optical transmittance of over 90% at a wavelength of 550 nm and a low sheet resistance of 50 Ω sq−1. Furthermore, the sheet resistance shows an excellent thermal and mechanical stability with a change of only about 2% in a bending test of 20 000 cycles or at a high temperature of 220 °C. This result shows that stacking graphene with stable 2D DL is a promising approach for graphene‐based next generation TCE.

Graphene growth on a copper surface via metal-catalyzed chemical vapor deposition has several advantages in terms of providing high-quality graphene with the potential for scale-up, but the product is usually inhomogeneous due to the inability to control the graphene layer growth. The non-uniform regions strongly affect the reliability of the graphene in practical electronic applications. Herein, we report a novel graphene transfer method that allows for the selective exfoliation of single-layer graphene from non-uniform graphene grown on a Cu foil. Differences in the interlayer bonding energy are exploited to mechanically separate only the top single-layer graphene and transfer this to an arbitrary substrate. The dry-transferred single-layer grapheme showed electrical characteristics that were more uniform than those of graphene transferred using conventional wet-etching transfer steps.