The advent of graphene opens up the research into two-dimensional (2D) material, which is considered as a revolutionary material in the future. Due to its unique geometric structure, graphene exhibits a series of exotic physical and chemical properties. Besides, single-element-based 2D materials (Xenes) have garnered tremendous interest. At present, 16 kinds of Xenes (silicene, borophene, germanene, phosphorene, tellurene, etc.) have been explored, mainly distributed in the third, fourth, fifth and sixth main groups. The current methods to prepare monolayer or few-layer 2D materials include epitaxy growth, mechanical exfoliation, and liquid phase exfoliation. Although two Xenes (aluminene and indiene) have not been synthesized due to the limitations of synthetic methods or stability of Xenes, other Xenes have been successfully realized by elaborately artificial design and synthesis. Focusing on elemental 2D materials, this review mainly summarizes the recently reported work about tuning the electronic, optical, mechanical, or chemical properties of Xenes via surface modifications achieved by controllable approaches (doping, adsorption, strain, intercalation, phase transition, etc.) to broaden the applications in various fields, including spintronics, electronics, optoelectronics, superconducting, photovoltaics, sensors, catalysis, and biomedicines. These advances in surface modification of Xenes have laid a theoretical and experimental foundation for the development of 2D materials and their practical applications in diverse fields.