With the development of 5G, Internet of Things, and smart home technologies, miniaturized and compact multi-antenna systems and multiple-input multiple-output (MIMO) antenna arrays have attracted increasing attention. Reducing the coupling between antenna elements is essential to improving the performance of such MIMO antenna system. In this work, we proposed a graphene-assembled, as an alternative material rather than metal, film-based MIMO antenna array with high isolation for 5G application. The isolation of the antenna element is improved by a graphene assembly film (GAF) frequency selective surface and isolation strip. It is shown that the GAF antenna element operated at 3.5 GHz has the realized gain of 2.87 dBi. The addition of the decoupling structure improves the isolation of the MIMO antenna array to more than 10 dB and corrects the antenna radiation pattern and operating frequency. The isolation between antenna elements with an interval of 0.4λ is above 25 dB. All experimental results show that the GAF antenna and decoupling structure are efficient devices for 5G mobile communication.