A new wide-angle and polarization-insensitive metasurface (MS) instead of traditional antenna is built as the primary ambient energy harvester in this paper. The MS is a two-dimensional energy harvesting array that is composed of subwavelength electrical small ring resonator that is working at 2.5 GHz (LTE/WiFi). In the case of different polarization and incidence angles, we demonstrate the metasurface can achieve high harvesting efficiency of 90%. The fabricated prototype of 9 × 9 MS energy harvesting array is measured, and the experimental results validate that the proposed MS has a good performance more than 80% of energy harvesting efficiency for arbitrary polarization and wide-angle incident waves. The good agreement of the simulation with the experiment results verifies the practicability and effectiveness of the proposed MS structure, which will provide a new source of supply in wireless sensor networks (WSN).