A method for preparing a green and high-efficiency composite flocculant, which uses plant fibrous waste and inorganic aluminum salts as raw materials, uses sodium hydroxide as an alkalizing agent, chloroacetic acid as an etherifying agent, and uses inorganic aluminum salts as a matrix basic material. Composite flocculant composed of natural organic matter and inorganic aluminum salt, the steps are as follows: 1) alkalinize plant fibrous waste with sodium hydroxide solution; 2) add chloroacetic acid aqueous solution for etherification; 3) finally add inorganic aluminum salt aqueous solution for Composite reaction to obtain a gray-brown liquid composite flocculant. The advantages of the present invention are: good flocculation effect, no secondary pollution, good ecological safety; simple preparation method, mild reaction conditions, easy to scale up to realize industrial production; good economic performance, low cost, wide source of synthetic raw materials, conforming to circular economy, Requirements for clean production; a wide range of applications, suitable for a variety of industrial wastewater and domestic wastewater, and even industrial water supply, and can further expand the scope of use by adjusting the formula ratio.