Owing to their excellent electronic, mechanical, and chemical properties, carbon nanotubes (CNTs) have been extensively investigated for various applications. [1,2] Vertically aligned CNT arrays, prepared by chemical vapor deposition (CVD) methods, are considered to be well suited for many of these applications. [3][4][5][6][7] The properties of the supporting substrates on which the nanotube films are grown often play a critical role in some of these applications. For example, nanotube arrays on conductive metallic substrates exhibit improved field emission properties, [8] whereas nanotubes on flexible polymer substrates [9] may be well suited for certain device applications. However, only a limited variety of substrate materials are compatible with nanotube CVD growth processes. Typically, the CVD growth temperature is higher than 600°C, which limits the use of many substrates. We have recently demonstrated the direct growth of aligned MWNTs on a metallic alloy using vapor-phase catalyst-delivery-assisted CVD. [8] The interaction between the catalyst and substrate is critical for nanotube growth. Si and quartz wafers are the two substrate materials most commonly used to grow CNTs by CVD. [5][6][7] Several applications require the transfer or deposition of nanotube arrays onto substrates other than the ones they are grown on. Recently, we have demonstrated the contact transfer of aligned CNT arrays onto conducting substrates using low-temperature soldering.[10] For many applications, it is desirable to develop a technique to obtain freestanding CNT films by direct peeling from a substrate without disturbing their aligned structure. [11][12][13] Owing to the weak Van der Waals forces stitching together the vertically aligned nanotube arrays, the direct mechanical removal of CNT films from substrates could damage the alignment of nanotubes in the films. CNT films grown on silica have been released from the substrate by chemical etching processes. [14] Chemical processes tend to contaminate the nanotube films thus precluding their use in certain applications. Moreover, these processes induce the formation of a foam-like structure [15] when the nanotube arrays come in contact with solvents. The detachment of nanotube films from substrates by means of the thermocapillary effect has been attempted using hot distilled water, [16] which also results in the formation of foam-like structures.Hence it is important to develop new techniques to obtain freestanding CNT films without disturbing or degrading the alignment of nanotubes. Here, we report a reliable self-releasing technique to directly prepare freestanding vertically aligned CNT films. Freestanding CNT films thus obtained from a single CVD run retain their alignment and structure and can be directly used for applications. Additionally, this novel technique facilitates the effective incorporation of CNT films into devices in various configurations for practical applications.The experimental process for the growth of freestanding nanotube films essentially involves t...