This study aims to understand the effects and mechanisms of length, diameter, and functional group of carbon nanotubes (CNTs) on rheological behaviors of cementitious composites. The experimental results show that the addition of CNTs decreases the flow index and increases the critical shear rate of cementitious composites. CNTs with a sub-micrometer length and small diameter endow cementitious composites with high yield stresses and minimum viscosities. Influenced by the high water absorption of hydroxylic groups, the minimum viscosity of cementitious composites with hydroxyl functionalized CNTs is larger than that of composites with pristine carbon nanotubes (p-CNTs). By contrast, the yield stress and minimum viscosity of cementitious composites with carboxyl functionalized CNTs are smaller than that of cementitious composites with p-CNTs at most contents due to the high dispersion induced by carboxyl groups. The effect mechanisms of CNTs on rheological behaviors can be attributed to adsorption effect and entanglement effect, which are closely related to length, diameter and functionalization groups of CNTs. The established minimum viscosity prediction model considering the influence of CNT physicochemical features can provide guidance for regulating the workability and hardened performance of CNTs modified cementitious composites.