Recent progress in Large Language Models (LLMs) has opened new avenues for solving complex optimization problems, including Neural Architecture Search (NAS). However, existing LLM-driven NAS approaches rely heavily on prompt engineering and domain-specific tuning, limiting their practicality and scalability across diverse tasks. In this work, we propose LM-Searcher, a novel framework that leverages LLMs for cross-domain neural architecture optimization without the need for extensive domain-specific adaptation. Central to our approach is NCode, a universal numerical string representation for neural architectures, which enables cross-domain architecture encoding and search. We also reformulate the NAS problem as a ranking task, training LLMs to select high-performing architectures from candidate pools using instruction-tuning samples derived from a novel pruning-based subspace sampling strategy. Our curated dataset, encompassing a wide range of architecture-performance pairs, encourages robust and transferable learning. Comprehensive experiments demonstrate that LM-Searcher achieves competitive performance in both in-domain (e.g., CNNs for image classification) and out-of-domain (e.g., LoRA configurations for segmentation and generation) tasks, establishing a new paradigm for flexible and generalizable LLM-based architecture search. The datasets and models will be released at https://github.com/Ashone3/LM-Searcher.