On account of unique characteristics, the integration of metal–organic frameworks as active materials in electronic devices attracts more and more attention. The film thickness, uniformity, area, and roughness are all fatal factors limiting the development of electrical and optoelectronic applications. However, research focused on ultrathin free‐standing films is in its infancy. Herein, a new method, vapor‐induced method, is designed to construct centimeter‐sized Ni3(HITP)2 films with well‐controlled thickness (7, 40, and 92 nm) and conductivity (0.85, 2.23, and 22.83 S m−1). Further, traditional transfer methods are tactfully applied to metal–organic graphene analogue (MOGA) films. In order to maintain the integrity of films, substrates are raised up from bottom of water to hold up films. The stripping method greatly improves the surface roughness Rq (root mean square roughness) without loss of conductivity and endows the film with excellent elasticity and flexibility. After 1000 buckling cycles, the conductance shows no obvious decrease. Therefore, the work may open up a new avenue for flexible electronic and magnetic devices based on MOGA.