The present invention provides a straw-based selective mercury removal material preparation method, which comprises: (1) carrying out a steam explosion treatment on straws, and then treating at a temperature of 400-800 DEG C under vacuumizing and nitrogen atmosphere; (2) placing the product obtained in the step (1) into a reductive sulfur group-containing mixing liquid, carrying out stirring mixing, filtering, and drying, wherein the reductive sulfur group-containing mixing liquid is a mixing liquid of ammonium thiocyanate, ammonium thiosulfate and thioglycolic acid; and (3) mixing the product obtained in the step (2) and sublimed sulfur, heating under vacuumizing and nitrogen introducing conditions to achieve a temperature of 450 DEG C, maintaining for 2 h, carrying out program heating to 600-1000 DEG C, maintaining the vacuumizing and nitrogen introducing for 2 h, cooling, and grinding so as to obtain the straw-based selective mercury removal material. The invention further provides the mercury removal material prepared through the method and applications of the mercury removal material in mercury removal. According to the present invention, the straw-based selective mercury removal material has advantages of high mercury adsorption capacity, high mercury removal rate, rapid mercury removal, high selectivity, cheap and easily available raw materials, simple and feasible preparation process, environmental protection, economy, and good application prospect.