A sustainable environment by decreasing fossil fuel utilization and anthropogenic greenhouse gases is a globally main goal due to climate change and serious air pollution. Carbon dioxide (CO2) is a heat-trapping (greenhouse) that is released into the earth’s atmosphere from natural processes, such as volcanic respiration and eruptions, as well as human activities, such as burning fossil fuels and deforestation. Due to this fact, underground carbon storage (UCS) is a promising technology to cut carbon emissions. However, there are some barriers to prevent UCS from applying globally. One of them is evaluating the feasibility of storage projects. Thus, the prediction accuracy of CO2 storage efficiencies may promote the attention of the community for UCS. In this study, we utilize the recent advances of swarm intelligence to develop a hybrid algorithm called AOSMA, employed to train the long short-term memory (LSTM). The developed swarm intelligence method (AOSMA) is an enhanced Aquila optimizer (AO) using the search mechanism of the slime mould algorithm (SMA). It is used to boost the prediction capability of the LSTM by optimizing its parameters. We considered two CO2 trapping indices, called residual trapping index (RTI) and solubility trapping index (STI). The evaluation experiments have shown that the AOSMA achieved significant results compared to the original AO and SMA and several swarm intelligence and optimization algorithms. The developed smart tools could use as a game changer to provide fast and accurate storage efficiency for projects that have similar parameters falling within the range of the database.