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Template wetting is simple, solution-based nanofabrication technique that has previously been demonstrated for a number of different polymers. Like other solution-based polymer processing methods, it is reasonable to expect that the choice of solvent will have a significant impact on the properties of the resulting structures. This work examines the impact of wetting solvent on the properties of poly(2-methoxy-5-2′-ethylhexyloxy-1,4-phenylenevinlyene) (MEH-PPV) nanotubules formed using this method. The strength of solvent−polymer interaction was found to positively correspond to the degree of polymer chain alignment in the resulting nanotubules. Alignment was indicated by the level of dichroism observed using polarized FTIR spectroscopy, with no preferential alignment observed when using the poorest solvent (chlorobenzene) and dichroic ratios greater than 10 observed when “good” solvents chloroform and tetrahydrofuran were employed. The degree of alignment in turn correlated to a greater effective conjugation length in the MEH-PPV nanotubules, indicated by a small red shift in the UV−vis absorption band. An even greater impact of solvent on hole mobility was observed, with the best solvent examined yielding a roughly 3 orders of magnitude greater hole mobility than the worst solvent studied in the nanotubules.