Dental caries, as the predominant global oral disease, remains a critical public health issue worldwide, particularly in socioeconomically disadvantaged communities. However, common caries prevention approaches (e.g., oral health education, mechanical plaque removal, and delivery of fluoride agents) are still insufficient for optimal caries management, and therefore, alternative regimens that can supplement existing strategies are highly warranted. Nanomaterials exhibit considerable potential in combating cariogenic pathogens and biofilms owing to their promising antimicrobial capacity, improved penetration into biofilms, targeted precision delivery, and versatile physicochemical properties. As unifunctional materials are limited in caries management, this review underscores the latest advancement in multifunctional anti-caries nanomaterials/nanomedicines. It highlights the cutting-edge materials developed or engineered to (i) incorporate diagnostic capabilities to prevent caries at an early stage, thus enhancing treatment efficiency, (ii) integrate mechanical "brushing" with anti-caries approaches to mechanochemically eradicate biofilms, (iii) exert antimicrobial/antibiofilm effects while preserving dental hard tissue. The current work also outlines future directions for optimizing nanosystems in the management of dental caries while emphasizing the need for innovative solutions to improve preventive and therapeutic efficacies.