The integration of Large Language Models (LLMs) with Neural Architecture Search (NAS) has introduced new possibilities for automating the design of neural architectures. However, most existing methods face critical limitations, including architectural invalidity, computational inefficiency, and inferior performance compared to traditional NAS. In this work, we present Collaborative LLM-based NAS (CoLLM-NAS), a two-stage NAS framework with knowledge-guided search driven by two complementary LLMs. Specifically, we propose a stateful Navigator LLM to guide search direction, a stateless Generator LLM to synthesize high-quality candidates, and a Coordinator module to orchestrate inter-LLM communication and manage evaluation processes. CoLLM-NAS efficiently guides the search process by combining LLMs' inherent knowledge of structured neural architectures with progressive knowledge from iterative feedback and historical trajectory. Experimental results on ImageNet and NAS-Bench-201 show that CoLLM-NAS surpasses existing NAS methods and conventional search algorithms, achieving new state-of-the-art results while significantly reducing search costs by 4--10. Furthermore, CoLLM-NAS consistently enhances the performance and efficiency of various two-stage NAS methods (e.g., OFA, SPOS, and AutoFormer) across diverse search spaces (e.g., MobileNet, ShuffleNet, and AutoFormer), demonstrating its excellent generalization.