that satisfy the growing needs for compact, small foot-print, highly efficient and broadband photonic and optoelectronic devices. In other words, the development between SA technologies and lasers is almost isochronous. By 1983, several mode-locked fiber lasers with actively doped fiber amplifiers were demonstrated largely driven by improvements in low-loss optical fibers. However, mode-locking with a dye SA was unstable in Nd:fibers at the time. [5] The early 1990s saw the semiconductor SA mirror (SESAM) invention which was a milestone in the realization of stable passive mode-locked pulses [6,7] and stable Q-switching. However, SESAM progress was impeded by the narrow operation bandwidth, challenging fabrication process, slow relaxation time and most importantly a weak mid-infrared (mid-IR) response. By contrast, 2D nanomaterials can possess shorter relaxation times with a highly efficient broadband response covering even the mid-IR. The fabrication methods, nonlinear optical properties and applications in optics, biomedicine, and other fields of 2D materials are shown in Figure 1. 2D materials are now the spotlight of SA research applications because of these unique properties along with stable quantum confinement, higher mechanical stability, and an inherently small-footprint. [8][9][10] Graphene has been a breakthrough 2D NLO material for a wide range of topics such as broadband optical modulation, [11] optical frequency mixing, [12] ultrafast laser generation, [13][14][15][16][17][18][19][20] and surface plasmonic. [21] Nevertheless, the development of this material is still limited to some extent [22] due to its innate gapless band structure and the weak electronic on/off ratio. Topological insulators (TIs) reveal a large modulation depth. However, the fabrication of TIs is complicated because of their two elements composition. [23][24][25] Transition metal dichalcogenides (TMDs) are unusable in the mid-IR region because of their large bandgaps. [26] In Group-VA monoelemental materials, black phosphorus (BP) is famous for the characteristic layer number dependent bandgap. [27][28][29][30][31][32][33][34][35] However, monolayer or fewlayer BP lacks of chemical stability at ambient conditions. [36,37] In addition, another Group-VA material, semiconducting antimonene, is relatively stable under ambient environment with a wide bandgap. [38] Bulk antimonene has great potential to become a TI as well as quantum spin Hall phase producer when the number of layers is under 22, respectively. [39] On top of this, antimonene is very chemically stable. It has good thermal conductivity, [40] high mobility, [41] excellent thermoelectric figure of merit, [42] and good optical properties, [43][44][45][46] which 2D materials have received significant attention from the scientific community due to their unique structures and excellent physical properties. A lot of applications are explored based on graphene, topological insulators, and transition metal dichalcogenides. With further development of 2D materials, other Group-VA...