Experimental protocols in organic synthesis specify not only the intended transformation but also an executable sequence of operations and conditions. While recent language models show strong chemistry knowledge, widely used evaluations remain less diagnostic of procedure-level decision making. In this setting, correctness requires consistent step ordering, feasibility under stated conditions, faithful entity-role grounding, and schema-parseable outputs that can be automatically validated against operational constraints. We present ChemReason-Bench, a human-validated benchmark for verifiable experimental procedure reasoning built on a structured representation with explicit placeholders and a unified schema, enabling automatic checks of many operational constraints. From 500 reactions, we instantiate 7306 benchmark tasks across six complementary formats: ordering, step validation, condition validation, schema-constrained completion, contrastive choice, and evidence-grounded rationalization. We further release a large-scale instantiation of the same templates for downstream adaptation studies, kept disjoint from the evaluation set. Using a unified evaluation protocol, we benchmark diverse open-source, proprietary, and domain-specific models and observe clear variation across the capability surface. We also report controlled adaptation experiments in the appendix, where supervised fine-tuning improves small models, preference optimization adds limited gains in our setting, and a gap remains to the strongest evaluated systems.

With the increasing interest in robotic synthesis in the context of organic chemistry, the automated extraction of chemical procedures from literature is critical. However, this task remains challenging due to the inherent ambiguity of chemical language and the high cost of human annotation required for developing reliable computer-aided extraction protocols. Here, we present ChemActor, a fully fine-tuned large language model (LLM), as a chemical executor to convert between unstructured experimental procedures and structured action sequences. We propose a sequential LLM-generated data framework to address the challenges of insufficient and low-quality annotated data. This framework integrates a data selection module that selects data based on distribution divergence, with a general-purpose LLM, to generate machine-executable actions from a single molecule input. Additionally, we introduce a novel multi-round LLMs circle review metric, which reflects the model’s advanced understanding of chemical experimental procedures. Extensive experiments on reaction-to-description (R2D) and description-to-action (D2A) tasks demonstrate that ChemActor, augmented by LLM-generated data, achieves state-of-the-art performance, outperforming the baseline model by 10%. The code is available at: https://github.com/Zhanghahah/ChemActor.