Self‐supporting mats of multi‐wall carbon nanotubes (MWCNT buckypaper) are an interesting and versatile nanotube application platform. In the course of our explorations in this field we prepared MWCNT buckypapers with a surface density of 5.6 mg·cm–2 and modified their surface with pyroelectric LiNbO3 and piezoelectric KNbO3 crystals. The temperature and pressure sensitivity of the prepared devices was different than that of the undoped buckypapers: the temperature response increased, the pressure response decreased compared to undoped MWCNT mats. The described method seems to open a new pathway for buckypaper functionalization. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)