During the last decade, worldwide attention of researchers has focused on nano-ceramic composites with superior mechanical behavior and improved reliability for structural applications. Here we report the development of a multi-layer composite (MLC) of tape cast nano zirconia with high failure energy. The MLC samples were fabricated by thermocompression of green tapes prepared from 3 mole % yttria stabilized zirconia (3-YSZ) powder with a primary crystallite size of 27 nm. Depending on the number of layers, the MLC samples exhibited failure energy (238.97 KJm −3 ) more than two times higher than that of the single tape (≈107 KJm −3 ) with a reasonably high bi-axial flexural strength (≈630 MPa), high hardness (≈ 13 GPa at 49 N), and indentation fracture toughness nearly four times as high as that of the single tape. In addition, these MLC materials showed the presence of a R-curve behavior.