Advances in nanotechnology and nanomaterials have attracted considerable interest and play key roles in scientific innovations in diverse fields. In particular, increased attention has been focused on carbon-based nanomaterials exhibiting diverse extended structures and unique properties. Among these materials, zero-dimensional structures, including fullerenes, carbon nano-onions, carbon nanodiamonds, and carbon dots, possess excellent bioaffinities and superior fluorescence properties that make these structures suitable for application to environmental and biological sensing, imaging, and therapeutics. This review provides a systematic overview of the classification and structural properties, design principles and preparation methods, and optical properties and sensing applications of zero-dimensional carbon nanomaterials. Recent interesting breakthroughs in the sensitive and selective sensing and imaging of heavy metal pollutants, hazardous substances, and bioactive molecules as well as applications in information encryption, super-resolution and photoacoustic imaging, and phototherapy and nanomedicine delivery are the main focus of this review. Finally, future challenges and prospects of these materials are highlighted and envisaged. This review presents a comprehensive basis and directions for designing, developing, and applying fascinating fluorescent sensors fabricated based on zero-dimensional carbon nanomaterials for specific requirements in numerous research fields.