In this communication, we report a scroll-like nanotubular structure found in an amorphous vinyl polymer of PS-Qu containing fluorescent tetraphenyl-quinoline (TP-Qu) pendant groups. By spin-casting dilute solution of PS-Qu, long nanoribbons with heights in correlated to the molecular width of TP-Qu pendant groups formed. On the contrast, single-, double-, and multiple-walled nanoscrolls are the major structures existing in the products from the slow-evaporation process. Presumably, scrolling of nanoribbons result in the scroll-like nanotubular structures with the resolved layer thickness in dimension close to molecular width of the TP-Qu pendant. Computer simulation on the single PS-Qu chain suggests the existence of a straight-chain backbone, with most of the vicinal 1,3-disubstituted TP-Qu groups positioned in near face-to-face arrangements. Intermolecular distances evaluated from the SAEDs were approached by the molecular dynamic of two straight-chain polymer backbones. Favorable π-π interactions among the vicinal 1,3-disubstitued TP-Qu groups are suggested to be a major factor leading to the straight-chain backbone and the observed nanoribbons and nanoscrolls.