Provided are a gas separation membrane which includes a gas separation layer formed to include a polyimide compound and in which the polyimide compound includes a repeating unit represented by the following Formula (I), a gas separation module, a gas separation device, and a gas separation method using the same. In Formula (I), R represents a group having a specific structure. R3 represents a specific substituent group. A1 to A3 represent a hydrogen atom or a specific substituent group, but all of A1 to A3 do not represent a hydrogen atom at the same time.In this case, at least one of R3, A1, A2, and A3 represents a specific polar group.