We demonstrate direct evidence that a single-crystal-like aragonite platelet is essentially assembled with aragonite nanoparticles. The aragonite nanoparticles are readily oriented and assembled into pseudo-single-crystal aragonite platelets via screw dislocation and amorphous aggregation, which are two dominant mediating mechanisms between nanoparticles during biomineralization. These findings will advance our understanding of nacre's biomineralization process and provide additional design guidelines for developing biomimetic materials.