A long-standing conflict concerning metastable β-titanium (Ti) alloys is that high strength can be achieved through precipitation strengthening of α-phase while plasticity is largely compromised and even lost completely. Such strength-plasticity trade-off severely limits their structural applications. Here, an attempt to address the issue has been made in Ti–6Cr–5Mo–5V–4Al (Ti6554) high-strength metastable β-Ti alloy. Heterogeneous β-structure is architected by partial static recrystallization (SRX) through properly manipulating solution treatment in the hot-rolled bars. The resulting microstructure is composed of the recrystallized ‘new’ equiaxed β-grains (βe) and the remnant elongated β-fibers (βf). This β-morphology dramatically affects the subsequent αs-precipitation behavior during the aging process. αs-precipitation is rather uniform throughout βf-grains because the pre-existing dislocations left by hot rolling provide copious nucleation sites. However, αGB-films are preferentially formed along βe-grain boundaries, which leads to a boundary-affect zone (BAZ) and thereby renders αs-precipitation in a size gradient from β-grain boundaries to grain interiors. As a result, an ultra-high strength of ∼1700 MPa is achieved whilst the ductility can be up to be 5% in the β-hetero aged samples, which is superior to the β-homo aged siblings that have the same strength level but fully succumb to macroscopic brittleness. The enhanced plasticity in the β-hetero aged samples originates from much better deformation compatibility conferred by the aged βf-grains. However, the soft feature of BAZ around βe-grain boundaries in the β-homo aged samples causes strain localization, which eventually induces intergranular brittle fracture. These findings provide an effective strategy for enhancing plasticity of high-strength metastable β-Ti alloys by structural design, where homogeneous αs-precipitates can be easily constructed by combining conventional thermomechanical processing and heat treatment.