We apply for continuation of our large-scale NAISS allocation to develop our research on advanced functional thin film materials at the international forefront. Our work integrates first-principles modeling, large-scale atomistic simulations, and method development with experimental synthesis and validation. The project brings together ~15 theoretical and as many experimental materials scientists, forming a tightly coupled computational–experimental research environment. Consistently over years, our use of NAISS resources results in a large body of publications in leading journals and significant scientific recognition, supported by major national and international funding. Computational usage remains consistently high and closely matched to allocations. Building on this momentum, we request an increased allocation to match the expanding scope and computational demands of our research. Our team is in the process of spinning out PIs for separate NAISS applications. This will promote diversity and renewal in research. We have done that in the recent past with the group of Professor Johanna Rosen at LiU. At the same time, we are careful to provide specific resource justifications for each present subproject not to burden the peer review process. Our workflows are being adapted to the coming transition in Swedish HPC infrastructure, where Tetralith is replaced by Arrhenius, and Dardel will be decommissioned in late 2026. In particular, we will increasingly exploit GPU-accelerated architectures on Arrhenius for VASP and machine-learning-potential-based simulations, while retaining targeted CPU usage for methods and potentials not yet compatible with GPU execution. Our main software tools are VASP and LAMMPS, both optimized for large-scale parallel execution and, where applicable, GPU acceleration. Machine-learning interatomic potentials (MLIPs) developed within our group enable simulations at unprecedented length and time scales, particularly for fracture, deformation, and defect evolution. In the coming period, we pursue three research directions: (1) Properties and phase stability of multifunctional materials, including novel 2D noble metals (like our recently discovered goldene, published in Nature Synthesis), nitrides, carbides, borides, high-entropy systems, and superlattices; (2) Method development for complex and disordered materials, advancing spin–lattice dynamics and MLIP frameworks for magnetic and disordered systems; and (3) Superconducting and energy-relevant materials, engineering superconducting properties and investigating radiation damage relevant to nuclear fusion. In brief, the project addresses key societal challenges related to energy production and storage, wear-resistant materials, magnetic technologies, and neutron detection. By integrating theory with experiment, we aim to deliver predictive materials design strategies and maintain Sweden’s leading position in computational materials science.