Post-training compression is essential for deploying large language models (LLMs) under tight resource constraints. Tensor decompositions have emerged as a promising direction, offering compact parameterizations well suited to Transformer weight structures. However, existing studies evaluate these methods in narrow settings, leaving unclear whether tensorization is effective at large-scale deployment. We systematically evaluate tensor compression across dense and MoE architectures, establishing performance trade-offs grounded in both empirical analysis and theoretical analysis. % We identify a fundamental mismatch between the shared subspaces assumed by tensor decompositions and the heterogeneous representations learned by modern LLMs, thereby delineating their practical limits and clarifying their viable role in large-scale deployment. We identify a fundamental mismatch between the shared subspaces assumed by tensor decompositions and the heterogeneous representations learned by modern LLMs, thereby delineating their practical limits that persist across an extensive range of mainstream dense and MoE deployment settings evaluated in this work. The code is available at https://github.com/brain-lab-research/TT-LLM.

Post-training quantization (PTQ) is essential for deploying LLMs under memory and bandwidth constraints. However, extreme low-bit quantization remains highly sensitive to activation outliers and anisotropic weight curvature. Existing incoherence-based PTQ methods mitigate this issue with fixed randomized Hadamard transforms (RHTs), which improve quantization robustness but cannot adapt the rotated basis to the layer, calibration distribution, or quantizer. We introduce HARP (Hadamard-preconditioned Adaptive Rotation Processor), a learnable structured two-sided orthogonal processor that replaces fixed Hadamard mixing while preserving exact full-precision equivalence. HARP represents each rotation as a product of sparse butterfly-like block-orthogonal stages, supports non-power-of-two dimensions through Mixed-Radix schedules, and initializes to the RHT processor up to a fixed permutation. Fitted only on calibration data, HARP adapts the quantization basis to each layer and backend. Across 2-4 bit settings on Llama models from 1B to 70B, HARP consistently improves perplexity and yields its clearest zero-shot gains at 2 bits; a 2-bit Qwen3-8B experiment shows the same transfer beyond the Llama family. HARP also preserves deployment efficiency: on Llama 2 7B at 2 bits, it reaches 128 tok/s, retaining 90% of RHT throughput (142 tok/s) and running approximately 2.1× faster than FP16 (61 tok/s).