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Polar topologies in ferroelectric oxides have received much attention for their potential applications in low-dimensional nano-electronic devices. However, a key challenge in this field is certainly that, how to modulate the transition and coexistence of different topological spin states, as it is essential for controlling topological spin structures and understanding the symbiosis of polarization and charge. Here, combining the dynamic modulation in thin film fabrication with nanodomain engineering, we have found a topological transition from the domains with irregular shapes by rapid cooling to regular striping domains in BiFeO 3 films after post-high temperature heat treatments. Further observations indicate that a series of multilayer topological domain groups are stabilized at the ferroelectric-insulator interface according to the polarization configurations at the atomic-scale resolution, where the charged domain walls and the topological domain provide favorable conditions for the domain modulation with regular arrangements and configurations. It is shown that the alternate arrangement of positive and negative bound charges allows 109° and 180° domains to delicately form the novel arrays with flux closure and vortices as characterized by atomic-resolved scanning transmission electron microscopy. For the piezoresponse force measurements, the clear evolution of ferroelectric domain patterns is observed with better piezoelectric properties achieved in thermally stabilized regular striping domains. This work provides new insights and guidance for artificially designing interface-dominated coexistence of polar topologies in monolayer ferroelectric films. [Display omitted] [ABSTRACT FROM AUTHOR]