As emission norms become stringent, the need for novel solutions to bring highly efficient technologies has gained importance. One of these methods is the use of alternative fuels and additives. Hydrogen enrichment of conventional fuels improves the combustion and emission characteristics of the base fuel. However, its application faces limitations such as storage, flammability, and transportation. Additionally, engine modifications are required to accommodate hydrogen supply and injection. Ammonia Borane (AB), a boron hydride, is an exceptional compound due to its high hydrogen storage capacity and has found application in many areas such as rocket fuels and fuel cells. The application of ammonia borane in internal combustion engines as a fuel additive is limited and is studied in the current work. A computational fluid dynamics engine model is developed and validated to predict the effect of AB addition on the performance and emission characteristics of gasoline-fueled engines. Results suggest that the addition of 5% AB decreases the in-cylinder pressure and temperature, reduces nitrogen oxides (NOx) and carbon monoxide (CO) emissions causes a delay in the onset of combustion. However, it can be predicted that ammonia borane can successfully be used as an additive for hydrogen enrichment of gasoline-fueled spark-ignited engines without any further engine modifications. Further, chemical reactions are modeled and recommendations to improve the mechanism of ammonia borane combustion are given. Current research can help understand the application of novel and nonconventional chemical compounds for efficient engine performance and improve understanding of combustion chemistry.