Bismuth sodium titanate (BNT) ceramics have outstanding strain responses but are unfavorable for applications in high-sensitivity displacement actuators due to large negative strain resulting from irreversible changes in their phase transition and domain structure. Here, (1-x)Bi0.50Na0.41K0.09TiO3-xNaNbO3 (BNKT-xNN) solid solutions were prepared to promote the strain properties through the strategy of modulating the phase boundary and domain structures. The introduction of sodium niobate could effectively regulate the relative content of tetragonal (P4bm) and rhombohedral (R3c) phases in the phase boundary region. The ferroelectric-to-relaxor phase transition (TF-R) was reduced and the ergodic relaxor (ER) state was nurtured at room temperature. An excellent zero-negative strain properties of S = 0.41% and d33* = 742 pm/V were achieved from the reversible transition between the ER and J u s t A c c e p t e d ferroelectric states under applied electric-field (x = 0.04). Additionally, understanding from domain states in piezoelectric force microscopy (PFM) and first-order reversal curves (FORC), the superior strain responses originated from the reversible inter-transformation of sub-stable macro-domains and polar nano-regions (PNRs) in the phase boundary. This study provides a new insight into the interplay between the evolution of phase boundary and domain structures and the strain properties of BNT-based ceramics.