The formation of specific interaction between poly(3,4-ethylenedioxythiophene) (PEDOT) and adenine (A), cytosine (C) and thymine (T) single stranded homonucleotides has been investigated, complementing our previous investigation on complexes formed by PEDOT and guanine (G) homonucleotide (B. Teixeira-Dias et al, Soft Matter, 2011, 7, 9922-9932). Results derived from UV-vis and FTIR spectroscopy suggest that A and, especially, C homonucleotides form adducts dominated by non-specific electrostatic interactions, while complexes with T homonucleotides show a behavior that differ from those found for A-, C- and G-containing systems. Results provided by molecular dynamics simulations were consistent with these experimental observations. Thus, specific interactions are much less abundant in A-and C-containing complexes than in those involving G. Moreover, simulations allowed us to detect a structural reorganization in the T-containing complexes, which occurs after their initial formation. This has been attributed to the optimization of electrostatic interactions rather than to the formation of new specific interactions, as was previously found in complexes with G. From the analysis of the interaction of the different nucleotides with an EDOT molecule it is concluded that the most stabilizing specific interaction corresponds to the formation of N-H center dot center dot center dot O-EDOT hydrogen bonds. Stabilization comes from electrostatic interactions, although the covalent contribution is non negligible ; Financial support from the MICINN and FEDER (MAT2009-09138, CTQ2011-23156/BQU, CTQ2011-25086/BQU, and UNGI08-4E-003) and Generalitat de Catalunya (2009SGR925, 2009SGR637 and XRQTC) is gratefully acknowledged. The authors are indebted to CESCA for computational facilities. B.T.D. is thankful for the financial support from the FPI grants program of the MICINN. J.P. also thanks the MICINN for the Ramon y Cajal contract. Support for the research of C.A. and M.S. was received through the prize "ICREA Academia" for excellence in research funded by the Generalitat de Catalunya