Titanium and titanium alloys have been widely applied in the manufacture of aircraft engines and aircraft skins, the mechanical properties of which have a crucial influence on the safety and lifespan of aircrafts. Based on nanotwinned titanium models with different twin boundary spacings, the impacts of different loadings and twin boundary spacings on the plastic deformation of titanium were studied in this paper. It was found that due to the different contained twin boundaries, the different types of nanotwinned titanium possessed different dislocation nucleation abilities on the twin boundaries, different types of dislocation–twin interactions occurred, and significant differences were observed in the mechanical properties and plastic deformation mechanisms. For the {101-2} twin, basal plane dislocations were likely to nucleate on the twin boundary. The plastic deformation mechanism of the material under tensile loading was dominated by partial dislocation slip on the basal plane and face-centered cubic phase transitions, and the yield strength of the titanium increased with decreasing twin boundary spacing. However, under compression loading, the plastic deformation mechanism of the material was dominated by a combination of partial dislocation slip on the basal plane and twin boundary migration. For the {101-1} twin under tensile loading, the plastic deformation mechanism of the material was dominated by partial dislocation slip on the basal plane and crack nucleation and propagation, while under compression loading, the plastic deformation mechanism of the material was dominated by partial dislocation slip on the basal plane and twin boundary migration. For the {1124} twin, the interaction of its twin boundary and dislocation could produce secondary twins. Under tensile loading, the plastic deformation mechanism of the material was dominated by dislocation–twin and twin–twin interactions, while under compression loading, the plastic deformation mechanism of the material was dominated by partial dislocation slip on the basal plane, and the product of the dislocation–twin interactions was basal dislocation. All these results are of guiding value for the optimal design of microstructures in titanium, which should be helpful for achieving strong and tough metallic materials for aircraft manufacturing.