In this study, the sol-gel stage co-precursor method was used to hydrophobically modify the gel and increase the content of alkali catalyst in the gel, thereby reducing the capillary force generated during ambient pressure drying and enhancing the strength of the gel skeleton. This improvement makes the gel skeleton structure not easy to destroy during the rapid drying process, thus greatly reducing the preparation time of atmospheric pressure drying, which could be as short as 10 h. It is worth mentioning that this method does not require extensive use of modifiers and organic solvents, so it has low cost, high efficiency, and broad industrial production application prospects. The experimental results show that the DDS/ZSA aerogel exhibits the lowest thermal conductivity (0.035 W m−1 K−1) when the dilute ammonia content is 5 ml. However, it should be noted that too low or too high an amount of dilute ammonia will lead to a decrease in aerogel performance, so it needs to be controlled within the appropriate range. In addition, the prepared aerogel has excellent hydrophobic properties with a contact angle greater than 140° and excellent thermal stability at 1000 °C, which can be used in harsh, humid, and high-temperature environments.