The commercially pure Ti (CP Ti) and equal-channel angular pressing (ECAP) processed Ti can contribute to the downsizing of medical devices with their superior mechanical properties and negligible toxicity. However, the ECAP-processed pure Ti has the risk of bacterial infection. Here, the coarse- and ultrafine-grained Ti substrates were surface-modified with molybdenum disulfide (MoS2) to improve the cell proliferation and growth with antibacterial effect for further dental applications. According to in vitro tests using the pre-osteoblast of MC3T3-E1 cell and a bacterial model of Escherichia coli (E. coli), MoS2 nanoflakes coated and ECAP-processed Ti substrates showed a significant increase in surface energy and singlet oxygen generation resulting in improved cell attachment and antibacterial effect. In addition, we confirmed the stability of the surface modified Ti substrates in a physiological solution and an artificial bone. Taken together, MoS2 modified and ECAP-processed Ti substrates might be successfully harnessed for various dental applications.