In this work, detailed studies of three different capillary-assisted techniques for the formations of large-scale multiwalled carbon-nanotube (MWNT)-based microstructures were presented. Using laser induced artificial vacancies, new insights into the effect of laser power, densities of MWNTs, and oxidation process dependencies for the creations of MWNT polygons were presented. With organized initiations, MWNT pillars were crafted out of MWNT arrays and 0.21 pL of water was found to produce sufficient force to bring about 14.7 mum deflections of a 9.19 x 9.19 x 24.1 mum(3) pillar, thereby allowing well-controlled formations of three-dimensional top-gathering MWNTs. Lastly, by twisting densified MWNT microbelts, 14 times improvements in resistivity as compared to undensified MWNT microwalls were achieved. Through prepatterning, the amount of twisting effect could be controlled, and this in turn allowed control of the resistance of the densified MWNT microwalls. These new insights and techniques presented could further encourage the use of self-organized MWNT structures with initiation as a flexible and viable route for the implementations of carbon-nanotube-based electronic devices.