In order to balance the strength and ductility of titanium matrix composites (TMCs), in-situ TiC/Ti composites with layered structures have been prepared by graphene oxides (GOs) electrophoretic deposition on pure Ti foils followed by spark plasma sintering (SPS) process. In order to further modifying the mechanical property, the sintered composites were subjected to cold rolling and annealing. The results show that GOs on the surface of Ti foil reacts with Ti matrix to form in situ TiC phases, thus forming TiC/Ti layered composites. With increasing deposition duration, the content of TiC distributed between Ti layers increases. After cold rolling and annealing, the grains of annealed composites are equiaxed, and the TiC still planarly distributed in the composites. The ultimate tensile strength (UTS) and the elongation (δ) of sintered material are 555 MPa and 15% respectively, while the UTS of annealed material is 568 MPa and the δ is 27%. Compared with sintered materials, annealed material achieves good strength-plasticity synergy. In addition, the strengthening and toughening mechanism of composites was discussed based on the analysis of microstructure and fracture behavior.