Deciphering the human visual experience through brain activities captured by fMRI represents a compelling and cutting-edge challenge in the field of neuroscience research. Compared to merely predicting the viewed image itself, decoding brain activity into meaningful captions provides a higher-level interpretation and summarization of visual information, which naturally enhances the application flexibility in real-world situations. In this work, we introduce MindSemantix, a novel multi-modal framework that enables LLMs to comprehend visually-evoked semantic content in brain activity. Our MindSemantix explores a more ideal brain captioning paradigm by weaving LLMs into brain activity analysis, crafting a seamless, end-to-end Brain-Language Model. To effectively capture semantic information from brain responses, we propose Brain-Text Transformer, utilizing a Brain Q-Former as its core architecture. It integrates a pre-trained brain encoder with a frozen LLM to achieve multi-modal alignment of brain-vision-language and establish a robust brain-language correspondence. To enhance the generalizability of neural representations, we pre-train our brain encoder on a large-scale, cross-subject fMRI dataset using self-supervised learning techniques. MindSemantix provides more feasibility to downstream brain decoding tasks such as stimulus reconstruction. Conditioned by MindSemantix captioning, our framework facilitates this process by integrating with advanced generative models like Stable Diffusion and excels in understanding brain visual perception. MindSemantix generates high-quality captions that are deeply rooted in the visual and semantic information derived from brain activity. This approach has demonstrated substantial quantitative improvements over prior art. Our code will be released.