3D printing of heterogeneous alloys holds promising application potentials in industry, especially in the field of aerospace. However, the relationship between the microstructure and mechanical properties of heterogeneous gradient titanium alloys produced by this technique, especially the micromechanical properties and mechanisms within the gradient zones, remains largely unexplored. In this study, we investigated the tensile micromechanical properties and deformation mechanism of 3D printed TC4/TC11 titanium alloy using the digital image correlation method in combination with scanning electron microscopy. The results show that this heterogeneous gradient titanium alloy possesses superior tensile properties. Furthermore, we elucidated the influence of microstructure and grain size on the alloy’s mechanical properties. Notably, an increased presence of secondary α phases and refined grain size were found to reduce the likelihood of microcrack initiation and propagation. Interestingly, all samples fractured on the TC4 side, with the microcracks predominantly extending at a 45° angle to the tensile direction. This observation underscores the necessity for optimizing the fabrication process of the TC4 alloy. Additionally, the strengthening mechanism of the gradient-bonded region of the alloy was also explored. The heterogeneous deformation-induced strengthening was identified as a key factor enhancing the strength of the dual alloyed zone. Collectively, this study provides valuable insights for optimizing the 3D printing process of heterogeneous gradient titanium alloys. It also lays a solid foundation for future investigation in this burgeoning field.