1,3-Butadiene (hereinafter referred to as butadiene), as an important organic intermediate in the chemical industry, has a wide range of uses in the petroleum and rubber industries. Using ethanol as raw material to produce butadiene can solve the non-renewable problem of raw materials, so it has received more and more attention. In this paper, catalysts were hydrothermally synthesized by using SBA-15 as the support, nitrate as the oxide precursor, and nitrogen-containing organic compounds as the additive. And then, the relationship between catalytic performance (ethanol conversion and butadiene yield) and the acid-base properties of catalysts was explored in the synthesis of butadiene from ethanol. Specifically, we used melamine (M), cyanuric acid (Ma), 1,10-phenanthroline (Pm), imidazole (Im), and 1,3,5-triazine (St) as nitrogen-containing additives for the preparation of Zn-Zr/SBA-15+X catalysts. Through the activity evaluation of the catalysts, the activities of ethanol dehydrogenation and dehydration, acetaldehyde condensation, and Meerwein-Ponndorf-Verley (MPV) reactions were calculated. Then, by analyzing the dependence of these activities and butadiene yield on the acidity and basicity (the strength and number of acidic/basic sites) of catalysts, we found that appropriate amounts of weak acid (0.022 mmol·g−1), moderate acid (0.078 mmol·g−1), moderate base (0.055 mmol·g−1), and strong base (0.056 mmol·g−1) are helpful for the ethanol dehydrogenation, whereas excess amount of weak acid and moderate acid will lead to the ethanol dehydration. Appropriate amounts of moderate acid (0.078 mmol·g−1) and moderate base (0.055 mmol·g−1) will favor the acetaldehyde condensation and MPV reactions. The butadiene yield is closely related to the activities of acetaldehyde condensation and MPV. The melamine-modified catalyst (Zn-Zr/SBA-15+M) has the optimum amounts of weak acid, moderate acid, moderate base, and strong base in accordance with the above quantities, resulting in the best catalytic performance: 99.5% conversion of ethanol, 65.5% selectivity of butadiene, and 0.45 gBD·gcat−1·h−1 of butadiene productivity.