Bio-inspired materials strategy seeks inspiration from nature for their use as models in the organization of advanced materials with embedded structural hierarchy. Biominerals are highly sophisticated interfacial materials and have functions integrated by self-assembly and mineralization of biomacromolecules. Polysaccharides, representing approximately three quarters of natural biomass resources, have the richness of structure, chemistry and actuation properties. They play critical roles in the organization and functional integration of biominerals, typical examples including chitin in lobster cuticle and nacre shells. Such materials can provide environmentally compatible solutions to some of the modern technological problems. Representative biominerals including nacre shells, lobster cuticle and diatom frustules, and some pertinent bio-inspired materials with salient structural functions are reviewed. The self-assembly and actuation properties of selected polysaccharides such as cellulose and alginate, and their inspiration to the design of advanced materials are covered. The concept of cooperative assembly of inorganic-polysaccharides interfacial materials is introduced, and representative advancement in bio-inspired functional integration by self-assembly and mineralization of polysaccharides are highlighted. It is hoped that this article will encourage further scientific investigations and invite more insightful view as how bio-inspired functional integration can be best achieved by self-assembly and mineralization of polysaccharides.