The moiré-pattern with slightly interlayer-twisted bilayer two-dimensional (2D) materials has recently been receiving substantial attention. One of the major characters for these intriguing structures is the appearance of low-energy ultra-flat bands and thus a package of new physics associated with strong electron correlation emerges. However, such new physics may become vague unless the twist-angle θ is sufficiently small such as θ ∼ 1°, making practical applications and control-flexibility hard to handle. In this work, we explore the possible flat-band moiré physics in recently concerned 2D bilayer α-In2Se3 which is antiferroelectric with sublayer out-of-plane (OP) polarizations, addressing the potential role of polarization-bound charges in modulation of electron–electron correlation and interlayer hybridization, based on the extensive first-principles calculations. On one hand, it is found that the low energy band becomes extremely flat in the bilayer α-In2Se3 moiré-pattern with relatively large twist-angle, e.g. θ = 13.17°, which is more easily accessible experimentally. On the other hand, the impact of the sublayer OP polarizations on the band structure is asymmetric, and the flattening effect is much more remarkable for the end-to-end polarization alignment but weaker for the head-to-head alignment. This work thus opens a broad roadmap for technological access to artificial fabrication of novel moiré-patterned 2D materials by means of low-dimensional ferroelectricity.