This chapter discusses the concept of human-centered large language models (LLMs). It explores both the opportunities and challenges involved in designing LLMs that are aligned with human values, highlighting the significance of human-centricity and reflecting on key considerations such as inclusivity, transparency, controllability, and sustainability. The chapter examines key challenges and how they arise across the LLM design lifecycle, advocating for an integrated approach that considers not only the development of the underlying models but also the design of the interfaces and interaction methods through which people engage with them. It provides an overview of current developments in the field and discusses key design principles and case studies of effective human-AI interaction. The chapter concludes by highlighting important trends and prospects in various sectors.