In this paper, a ϵ-negative metasurface superstrate is proposed for mutual coupling reduction of large antenna arrays. Unlike the previous decoupling metasurface works that are mostly confined to two-ports antennas, the proposed decoupling superstrate can be extended to massive multiple-input multiple-output (MIMO) systems. A 4 × 4 antenna array is used as an example to illustrate the decoupling performance of the proposed metasurface. With the decoupling metasurface, the worst mutual coupling of the antenna array is improved by 8 dB over the operation bandwidth with a maximum mutual coupling reduction of 25 dB. Moreover, the decoupling metasurface also help restore the radiation patterns, bring down the active voltage sanding wave ratio, and broaden the bandwidth of the array.