A new bulky pyrene-derived elongated cross-shaped organic scaffold was successfully incorporated into a highly porous, non-interpenetrated square-grid copper(II)-organic framework material with the unprecedentedly huge dimensions of 25.5 x 25.5 angstrom(2), while the layer-to-layer NH center dot center dot center dot N interaction leads to a unique hydrogen-bonded 6(4).8(2)-nbo net.