In this paper, we propose the CrossNAS framework, an automated approach for exploring a vast, multidimensional search space that spans various design abstraction layers-circuits, architecture, and systems-to optimize the deployment of machine learning workloads on analog processing-in-memory (PIM) systems. CrossNAS leverages the single-path one-shot weight-sharing strategy combined with the evolutionary search for the first time in the context of PIM system mapping and optimization. CrossNAS sets a new benchmark for PIM neural architecture search (NAS), outperforming previous methods in both accuracy and energy efficiency while maintaining comparable or shorter search times.