Tetrathiafulvalene-based molecular conductors, namely [TTF][TCNQ], (TTF) 6 [N(C 2 H 5 ) 4 ](HPM 12 O 40 ) (M ~W, Mo), and TTF[Ni(dmit) 2 ] 2 have been processed as thin films on microrough (001)-oriented silicon substrates using three different techniques. CVD-grown [TTF][TCNQ] deposits consist of platelets (10 6 5 mm) and filaments (diameter y1 mm). CN stretching modes in the infrared spectrum and CC stretching modes in the Raman spectrum are in agreement with a charge transfer of y0.6 from the TTF donor to the TCNQ acceptor. The N(1s) photoelectron spectrum confirms the presence of a reduced tetracyanoquinodimethane moiety. The films exhibit a semiconducting behaviour with a room-temperature conductivity of y0.4 S cm 21 . Deposits of (TTF) 6 [N(C 2 H 5 ) 4 ](HPW 12 O 40 ) are electrodeposited on microrough Si(001) at constant current from TTF and [N(C 2 H 5 ) 4 ] 3 (PW 12 O 40 ) in acetonitrile solution. The films are made of stacked sheets (5 v thickness v 25 mm). Vibrational spectra, conductivity measurements and magnetic susceptibility data are similar to those obtained on single crystals of (TTF) 6 [N(C 2 H 5 ) 4 ](HPW 12 O 40 ) grown on a platinum electrode. Thin films of TTF[Ni(dmit) 2 ] 2 are grown on microrough Si(001) by an adsorption process in organic solution. The deposits are characterized by Raman micro-probe and exhibit a pseudo-metallic behaviour with a room-temperature conductivity of about 2 S cm 21 .

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