石墨烯因其独特的电子性质在纳米电子学、功能材料、生物、能源等领域展现出了丰富的应用前景.第一原理计算研究可以对石墨烯材料进行有效的电子功能化设计,从而为实验上进行有目的合成或表征提供可靠的理论依据和指导.本文从晶格缺陷、边缘功能化、表面吸附掺杂和界面调控等4个方面总结了对石墨烯材料进行功能调制的主要理论进展.同时,也回顾了一些相关的实验进展. Due to its unique electronic properties, graphene has been widely used in many fields such as nanoelectronics, functional materials, biology, energy, etc. The first principle computational study can effectively design electronic functionalization of graphene materials, Which provides a reliable theoretical basis and guidance for the purpose of synthesis or characterization.This paper summarizes the main theoretical progress of functional modulation of graphene materials from four aspects: lattice defects, edge functionalization, surface adsorption doping and interface control. At the same time, some relevant experiments are also reviewed.