Reverse osmosis (RO) membranes are widely used in the field of water treatment. However, there are inevitably various fouling problems during long-term use. Surface engineering of RO membranes, such as hydrophilic modification, has attracted broad attention for improving the anti-fouling performance. In this work, we constructed a green biomimetic composite modification layer on the surface of polyamide membranes using a dopamine (DA)/tannic acid (TA) co-deposited layer to bridge the polyamide surface and hydrophilic phytic acids (PhA). The DA/TA interlayer could firmly adhere to the RO membranes, reducing the aggregation of DA and providing abundant phenolic hydroxyl sites to graft PhA. Meanwhile, the anchored PhA molecule bearing six phosphate groups could effectively improve the superficial hydrophilicity. The membranes were characterized by the SEM, AFM, XPS, water contact angle test, and zeta potential test. After surface modification, the hydrophilicity, smoothness, and surface electronegativity were enhanced obviously. The flux and rejection of the virgin membrane were 76.05 L·m−2·h−1 and 97.32%, respectively. While the modified D2/T4-PhA membrane showed decent permeability with a water flux of 57.37 L·m−2·h−1 and a salt rejection of 98.29%. In the dynamic fouling test, the modified RO membranes demonstrated enhanced anti-fouling performance toward serum albumins (BSA), sodium alginates (SA), and dodecyl trimethyl ammonium bromides (DTAB). In addition, the modified membrane showed excellent stability in the 40 h long-term test.