Aligning large language models (LLMs) typically aim to reflect general human values and behaviors, but they often fail to capture the unique characteristics and preferences of individual users. To address this gap, we introduce the concept of Personality Alignment. This approach tailors LLMs' responses and decisions to match the specific preferences of individual users or closely related groups. Inspired by psychometrics, we created the Personality Alignment with Personality Inventories (PAPI) dataset, which includes data from over 320,000 real subjects across multiple personality assessments - including both the Big Five Personality Factors and Dark Triad traits. This comprehensive dataset enables quantitative evaluation of LLMs' alignment capabilities across both positive and potentially problematic personality dimensions. Recognizing the challenges of personality alignments—such as limited personal data, diverse preferences, and scalability requirements—we developed an activation intervention optimization method. This method enhances LLMs' ability to efficiently align with individual behavioral preferences using minimal data and computational resources. Remarkably, our method, PAS, achieves superior performance while requiring only 1/5 of the optimization time compared to DPO, offering practical value for personality alignment. Our work paves the way for future AI systems to make decisions and reason in truly personality ways, enhancing the relevance and meaning of AI interactions for each user and advancing human-centered artificial intelligence. The dataset and code are released at https://github.com/zhu-minjun/PAlign.