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Laser Hot Wire (LHW) Directed Energy Deposition (DED) Additive Manufacturing (AM) processes are capable of manufacturing parts with a high deposition rate. There is a growing research interest in replacing large cast Nickel Aluminum Bronze (NAB) components using LHW DED processes for maritime applications. Understanding thermomechanical behavior during LHW DED of NAB is a critical step towards the production of high-quality NAB parts with desired performance and properties. In this paper, finite element simulations are first used to predict the thermomechanical time histories during LHW DED of NAB test coupons with an increasing geometric complexity, including single-layer and multilayer depositions. Simulation results are experimentally validated through in situ measurements of temperatures at multiple locations in the substrate as well as displacement at the free end of the substrate during and immediately following the deposition process. The results in this paper demonstrate that the finite element predictions have good agreement with the experimental measurements of both temperature and distortion history. The maximum prediction error for temperature is 5% for single-layer samples and 6% for multilayer samples, while the distortion prediction error is about 12% for single-layer samples and less than 4% for multilayer samples. In addition, this study shows the effectiveness of including a stress relaxation temperature at 500 °C during FE modeling to allow for better prediction of the low cross-layer accumulation of distortion in multilayer deposition of NAB.