Vertically aligned carbon nanotube (VACNT) arrays grown on quartz particles were produced in large amount via a floating catalysis process. Initially fast synchronous growth of VACNT arrays was observed, which is independently of the irregular shape and rough surface of the quartz particles. However, long VACNT arrays cracked and scattered anisotropically, depending on the irregular particles. The VACNTs have inner diameter of about 8.0 nm and relatively wide outer diameter distribution with a mean value of 36 nm. The outer diameter of CNTs, however, can be further decreased to 19 nm by tuning carbon source and concentration of catalyst precursor. The VACNTs have a high purity up to 97%. This work presents a simple way for controllable continuous production of VACNT array in large scale.