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Microstructure and composite mechanism of polymer modified cement (PMC) and mortar have been studied. Microstructure of PMC was observed by cryo-SEM. Dispersed polymer particles were observed in the hardened body. Polymer films were observed on the surface of hardened samples and at the interface of cement or aggregate in PMC. The bending strength of PMC was increased by the action of soft polymer particles in the hardened body. Adhesive strength of PMC was improved by the formation of polymer films. Both the particle dispersion of polymer and the formation of polymer films are useful as the composite mechanism of PMC.