This Study Aims to Explore Bond Capacity between Monolayer Graphene and Cementitious Composites for the First Time through a Pullout Test. the Low-Pressure Chemical Vapor Deposition Method Was Used to Synthesize Monolayer Graphene on the Copper Substrate to Be Embedded in the Mortar Made by the Briquette Mold. the Bond Capacity between Them Was Higher Than the Tensile Strength of the Copper Sheet with As-Grown Monolayer Graphene on the Surface Since All Specimens Failed in Fracture with Embedment Length of More Than 30 Mm. the Monolayer Graphene Enhanced the Copper Tensile Fracture Stress and Normalized Energy during the Test as the Copper Sheet Width Increased. This Short Communication Explores a New Path to Quantify the Bond between the Monolayer Graphene and the Mortar to Promote the Understanding of the Behavior of Graphene-Enhanced Cementitious Composites.