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In the “post‐Moore's Law” era, new materials are highly expected to bring next revolutionary technologies in electronics and optoelectronics, wherein 2D materials are considered as very promising candidates beyond bulk materials due to their superiorities of atomic thickness, excellent properties, full components, and the compatibility with the processing technologies of traditional complementary metal‐oxide semiconductors, enabling great potential in fabrication of logic, storage, optoelectronic, and photonic 2D devices with better performances than state‐of‐the‐art ones. Toward the massive applications of highly integrated 2D devices, large‐size 2D single crystals are a prerequisite for the ultimate quality of materials and extreme uniformity of properties. However, at present, it is still very challenging to grow all 2D single crystals into the wafer scale. Therefore, a systematic understanding for controlled growth of various 2D single crystals needs to be further established. Here, four key aspects are reviewed, i.e., nucleation control, growth promotion, surface engineering, and phase control, which are expected to be controllable at different periods during the growth. In addition, the perspectives on designed growth and potential applications are discussed for showing the bright future of these advanced material systems of 2D single crystals.

The electrochemical conversion of CO2 to valuable fuels is a plausible solution to meet the soaring need for renewable energy sources. However, the practical application of this process is limited by its poor selectivity due to scaling relations. Here we introduce the rational design of the monolayer hexagonal boron nitride/copper (h-BN/Cu) interface to circumvent scaling relations and improve the electrosynthesis of CH4. This catalyst possesses a selectivity of >60% toward CH4 with a production rate of 15 μmol·cm–2·h–1 at −1.00 V vs RHE, along with a much smaller decaying production rate than that of pristine Cu. Both experimental and theoretical calculations disclosed that h-BN/Cu interfacial perimeters provide specific chelating sites to immobilize the intermediates, which accelerates the conversion of *CO to *CHO. Our work reports a novel Cu catalyst engineering strategy and demonstrates the prospect of monolayer h-BN contributing to the design of heterostructured CO2 reduction electrocatalysts for sustainable energy conversion.

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