Chirality is a unique phenomenon in nature. Chiral interactions play an important role in biological and physiological processes, which provides much inspiration for scientists to develop chiral materials. As a breakthrough from traditional materials, biointerface materials based on chiral polymers have attracted increasing interest over the past few years. Such materials elegantly combine the advantages of chiral surfaces and traditional polymers, and provide a novel solution not only for the investigation of chiral interaction mechanisms but also for the design of biomaterials with diverse applications, such as in tissue engineering and biocompatible materials, bioregulation, chiral separation and chiral sensors. Herein, we summarize recent advances in the study of chiral effects and applications of chiral polymer-based biointerface materials, and also present some challenges and perspectives. Chirality is a unique phenomenon in nature. Chirality play an important role in biological and physiological processes, which allows much inspiration for scientists to develop chiral materials. As a breakthrough from traditional materials, biointerface materials based on chiral polymers have attracted increased interest over the past few years. Such materials elegantly combine the advantages of chiral surfaces and traditional polymers, and provide a novel solution not only for the investigation of chiral interaction mechanisms but also for the design of biomaterials with diverse applications, such as as in tissue engineering and biocompatible materials Herein, we summarize recent advances in the study of chiral effects and applications of chiral polymer-based biointerface materials, and also present some challenges and perspectives.