Target synthesis of metal organic nanotubes (MONTs) through a classic "rolling-up" mechanism remains a big challenge for coordination chemists. In this work, we report three 2D lamellar compounds and one (4,0) zigzag MONT based on a common honeycomb coordination skeleton. Our synthetic strategy toward sheet/tube superstructure transformation is to asymmetrically modify the inter-layer interactions by gradually increasing the size of the amine templates. Eventually, to relieve the surface tension of individual layers and to enhance surface areas and optimize host guest interactions to accommodate bigger guests, spontaneous rolling up to form a tubular structure was achieved.