Phyllosilicates, or sheet silicates, are an important group of minerals that include micas, chlorite, serpentine, talc and so on. Many transient metals can be incorporated into phyllosilicate structure like Ni, Co and Cu. Moreover, the high thermal and hydrothermal stability enable them to be applied for either gas reaction at high temperature or liquid reaction at low temperatures, making it a promising candidate of precursor of supported metal catalysts for certain reactions. Due to the unique layered structure, phyllosilicate-derived catalysts exhibit excellent catalytic performance for chemical, environmental and energy-related catalysis. In this review, we presented the preparation, characterization and catalytic applications of phyllosilicates. This review is mainly divided into five sections: (1) a general introduction to phyllosilicates, (2) synthesis of phyllosilicate material with various morphology, (3) characterizations applied to phyllosilicates, (4) catalytic applications of phyllosilicates, (5) summary and outlooks. We expected this review could help researchers understand more on phyllosilicate materials and lead more effort into the research of phyllosilicate-related catalysts.