Graphene and the following derivative 2D materials have been demonstrated to exhibit rich distinct optoelectronic properties, such as broadband optical response, strong and tunable light–mater interactions, and fast relaxations in the flexible nanoscale. Combining with optical platforms like fibers, waveguides, grating, and resonators, these materials has spurred a variety of active and passive applications recently. Herein, the optical and electrical properties of graphene, transition metal dichalcogenides, black phosphorus, MXene, and their derivative van der Waals heterostructures are comprehensively reviewed, followed by the design and fabrication of these 2D material‐based optical structures in implementation. Next, distinct devices, ranging from lasers to light emitters, frequency convertors, modulators, detectors, plasmonic generators, and sensors, are introduced. Finally, the state‐of‐art investigation progress of 2D material‐based optoelectronics offers a promising way to realize new conceptual and high‐performance applications for information science and nanotechnology. The outlook on the development trends and important research directions are also put forward.

Soliton frequency combs generate equally-distant frequencies, offering a powerful tool for fast and accurate measurements over broad spectral ranges. The generation of solitons in microresonators can further improve the compactness of comb sources. However the geometry and the material’s inertness of pristine microresonators limit their potential in applications such as gas molecule detection. Here, we realize a two-dimensional-material functionalized microcomb sensor by asymmetrically depositing graphene in an over-modal microsphere. By using one single pump, spectrally trapped Stokes solitons belonging to distinct transverse mode families are co-generated in one single device. Such Stokes solitons with locked repetition rate but different offsets produce ultrasensitive beat notes in the electrical domain, offering unique advantages for selective and individual gas molecule detection. Moreover, the stable nature of the solitons enables us to trace the frequency shift of the dual-soliton beat-note with uncertainty <0.2 Hz and to achieve real-time individual gas molecule detection in vacuum, via an optoelectronic heterodyne detection scheme. This combination of atomically thin materials and microcombs shows the potential for compact photonic sensing with high performances and offers insights toward the design of versatile functionalized microcavity photonic devices.