A selection of bolaamphiphilic perylene bisimides (PBI) were prepared from the reaction of perylenetetracarboxylic dianhydride with α-amino acids. These molecules were obtained in good yield using a simple synthetic protocol and avoiding the need for complex purification methods, a major advantage for future applications. Carbon nanotubes (CNT) were dispersed in an aqueous solution of the PBI, buffered at pH 7, and the suspension was studied by absorption and emission spectroscopy. PBI functionalized with Boc-lysine and phenylalanine led to an excellent suspension of CNT in water, stable for at least 24 h at room temperature. Theoretical calculations were used to support and explain the experimental observations.