In recent years,structure design and predictions based on global optimization approach as implemented in CALYPSO software have gained great success in accelerating the discovery of novel two-dimensional (2D) materials.Here we high-light some most recent research progress on the prediction of novel 2D structures,involving elements,metal-free and metal-containing compounds using CALYPSO package.Particular emphasis will be given to those 2D materials that exhibit unique electronic and magnetic properties with great potentials for applications in novel electronics,optoelectronics,magnetronics,spintronics,and photovoltaics.Finally,we also comment on the challenges and perspectives for future discovery of multi-functional 2D materials.