A novel cell-accumulation technique has been developed using highly biocompatible nanofilms by layer-by-layer assembly for the rapid construction of thick layered tissues with a well-controlled layer number and thickness. Furthermore, 3D tissues with highly developed blood capillary networks (over 1 cm(2) of layered tissues) were also constructed by sandwiching endothelial cells between the layered tissues. Such a simple and rapid methodology would be useful for tissue engineering and drug assessment.