The invention provides a method of preparing chestnut shell brown pigment by ultra-micronization in cooperation with pulsed electric field, comprising the steps of (1), cleaning, washing and drying chestnut shells and then primarily crushing the chestnut shells; (2), adding coarse chestnut shell powder into an ultra-micronization apparatus for wall breaking to obtain chestnut shell superfine powder; (3), using ethanol solution as an extracting solvent to extract the chestnut shell superfine powder by the aid of a pulsed electric field treating device, filtering, and combining double extracts to obtain pigment extract; (4), concentrating the pigment extract under reduced pressure to 1 / 3 of the original size, and carrying out alcohol precipitation, solid-liquid separation, concentration and drying to obtain the chestnut shell brown pigment that is powdery. The ultra-micronization and pulsed electric field treating techniques are combined, no heating is required to provide quick and complete dissolution of the chestnut shell pigment, extracting time and energy can be greatly saved, and the method has the advantages of rich material sources, low extracting temperature, high product yield is high, short treatment time, good operational simplicity and the like; the obtained chestnut shell brown pigment has high color intensity, good water-solubility, stable quality, safety with no toxicity and is worthy of practical production and conversion and practical popularization and application.