Large language models (LLMs) have revolutionized natural language processing, albeit at the cost of immense memory and computation requirements. Post-training quantization (PTQ) is becoming the de facto method to reduce the memory footprint and improve the inference throughput of LLMs. In this work, we aim to push the upper limit of LLM PTQ by optimizing the weight rounding parameters with the block reconstruction technique, a predominant method in previous vision models. We propose TesseraQ, a new state-of-the-art PTQ technique, to quantize the weights of LLMs to ultra-low bits. To effectively optimize the rounding in LLMs and stabilize the reconstruction process, we introduce progressive adaptive rounding. This approach iteratively transits the soft rounding variables to hard variables during the reconstruction process. Additionally, we optimize the dequantization scale parameters to fully leverage the block reconstruction technique. We demonstrate that TesseraQ can be seamlessly integrated with existing scaling or clipping-based PTQ algorithms such as AWQ and OmniQuant, significantly enhancing their performance and establishing a new state-of-the-art. For instance, when compared to AWQ, TesseraQ improves the wikitext2 perplexity from 14.65 to 6.82 and average downstream accuracy from 50.52 to 59.27 with 2-bit weight-only quantization of LLaMA-2-7B. Across a range of quantization schemes, including W2A16, W3A16, W3A3, and W4A4, TesseraQ consistently exhibits superior performance.