Two-dimensional materials are considered to be promising for next-generation electronic and energy devices. However, the limited availability of 2D materials hinders their applications. Herein, we employed high-throughput computation to discover new 2D materials by cleaving the bulk and to investigate their electronic, thermoelectric, and optoelectronic properties. Using our database containing 810 structures of chalcogenides ABX3 (A or B = Al, Ga, In, Si, Ge, Sn, P, As, Sb, and Bi; X = S, Se, and Te), we identified 204 new 2D compounds promising for experimental preparation according to the exfoliation energy. Notably, 96 of them are more easily exfoliated than graphene, 52 compounds show higher Seebeck coefficients than Bi2Te3 at 300 K, and 20 compounds have power factors beyond 2 × 10-3 Wm-1 K-2 at 900 K. Also, 6 new compounds exhibit high theoretical photovoltaic efficiency exceeding 30%. Our findings expand the 2D materials family and provide new 2D compounds for sustainable thermoelectric and optoelectronic energy applications.