Liquid Organic Hydrogen Carriers (LOHCs) have emerged as a promising solution for hydrogen storage, off ering high hydrogen

storage capacity, reversibility, thermal stability, and compatibility with existing infrastructures. Despite their potential,

LOHC systems face signifi cant challenges, including the need for specialized carriers and catalysts for effi cient hydrogen

storage and release. This review emphasizes the importance of computational analysis in overcoming these challenges.

We summarize the computational accuracy of estimating dehydrogenation enthalpy for the carrier materials and explore

molecular tuning strategies to enhance the dehydrogenation properties. In addition, we review computational studies that

have investigated the impacts of catalytic adsorption/desorption and kinetic properties on the catalytic performance as well

as catalyst design methods in terms of the geometry of active metal species, second metals, promoters, heterolytic hydrogen

generation, and hydrogen spillover. This review further addresses the current challenges in LOHC systems, and then suggests

future computational research directions to improve their effi ciency and viability.