The rapid advancements in Large Language Models (LLMs) have revolutionized various natural language processing tasks. However, the substantial size of LLMs presents significant challenges in training or fine-tuning. While parameter-efficient approaches such as low-rank adaptation (LoRA) have gained popularity, they often compromise performance compared to full-rank fine-tuning. In this paper, we propose Outlier-weighed Layerwise Sampled Low-Rank Projection (OwLore), a new memory-efficient fine-tuning approach, inspired by the layerwise outlier distribution of LLMs, which dynamically samples pre-trained layers to fine-tune instead of adding additional adaptors. We first interpret the outlier phenomenon through the lens of Heavy-Tailed Self-Regularization theory (HT-SR), discovering that layers with more outliers tend to be more heavy-tailed and consequently better trained. Inspired by this finding, OwLore strategically assigns higher sampling probabilities to layers with more outliers to better leverage the knowledge stored in pre-trained LLMs. To further mitigate the memory demands of fine-tuning, we integrate gradient low-rank projection into our approach, which facilitates each layer to be efficiently trained in a low-rank manner. By incorporating the efficient characteristics of low-rank and optimal layerwise sampling, OwLore significantly improves the memory-performance trade-off in LLM pruning. Our extensive experiments across various architectures, including LLaMa2, LLaMa3, and Mistral, demonstrate that OwLore consistently outperforms baseline approaches, including full fine-tuning. Specifically, it achieves up to a 1.1% average accuracy gain on the Commonsense Reasoning benchmark, a 3.0% improvement on MMLU, and a notable 10% boost on MT-Bench, while being more memory efficient. OwLore allows us to fine-tune LLaMa2-7B with only 21GB of memory.