Mapping computations to processors and assigning data to memory are critical for maximizing performance in parallel programming. These mapping decisions are managed through the development of specialized low-level system code, called mappers, crafted by performance engineers. Each mapper is tailored to a specific application and optimized for the underlying machine architecture, a process that requires days of refinement and tuning from an expert. Despite advances in system research, automating mapper generation remains a challenge due to the complexity of making millions of decisions to find the optimal solution and generate the solution as code. We introduce an approach that leverages recent advances in LLM-based optimizers for mapper design. In under ten minutes, our method automatically discovers mappers that surpass human expert designs in scientific applications by up to 1.34X speedup. For parallel matrix multiplication algorithms, our mapper achieves up to 1.31X of the expert-designed solution. To achieve this, we simplify the complexity of low-level code generation by introducing a domain-specific language (DSL) that abstracts the low-level system programming details and defines a structured search space for LLMs to explore. To maximize the application performance, we use an LLM optimizer to improve an agentic system that generates the mapper code. As a result, this approach significantly reduces the workload for performance engineers while achieving substantial performance gains across diverse applications. Finally, our results demonstrate the effectiveness of LLM-based optimization in system design and suggest its potential for addressing other complex system challenges.