The deployment of large language models (LLMs) is frequently hindered by prohibitive memory and computational requirements. While quantization mitigates these bottlenecks, maintaining model fidelity in the sub-1-bit regime remains a persistent challenge. In this paper, we introduce LittleBit, a novel framework for extreme LLM compression. We target quantization rates as low as $0.1$ bits per weight (BPW), achieving a memory reduction of approximately $31\times$, which effectively compresses Llama2-13B to under $0.9$ GB. We represent weights via low-rank latent matrix factorization and subsequently binarize the resulting factors. To counteract the information loss inherent to such drastic precision reduction, we integrate a multi-scale compensation mechanism that learns importance parameters across row, column, and latent dimensions. Two primary contributions enable effective training: Dual Sign-Value-Independent Decomposition (Dual-SVID) for quantization-aware training (QAT) initialization, and Residual Compensation to minimize approximation errors. Extensive experiments confirm the superiority of LittleBit in the sub-1-bit domain; for instance, our method at $0.1$ BPW surpasses the performance of leading techniques operating at $0.7$ BPW on Llama2-7B. We establish a new size-performance trade-off -- unlocking a potential $11.6\times$ inference speedup relative to FP16 -- and render powerful LLMs practical for resource-constrained environments. Our code is available at https://github.com/SamsungLabs/LittleBit.