Since the discovery of carbon nanotubes (CNTs) in 1991, a fundamental question still remained on how to control morphologically the synthesis of CNTs. This task has always been a challenge. In this paper, we report the results that we have published previously with the aim of sharing the possible controlled synthesis approach via this novel production method. Findings demonstrated that various CNTs could be synthesized by using specially developed supported catalysts from the catalytic decomposition of methane. These synthesized CNTs include carbon nanofibres, single-walled and multi-walled CNTs, Y-junction CNTs and CNTs with special morphologies. It was also revealed that catalyst composition and reaction parameters played an important role in controlling the morphology and type of CNTs formed. The synthesis of CNTs with various morphologies is important because this can enrich the nanostructures of the carbon family. This finding also provides useful data for better understanding of the parameters that govern the growth mechanism of CNTs which may be required in the near future for enhanced controlled synthesis of CNTs.