Understanding of the exotic quantum phenomena in bulk bismuth beyond its ultraquantum limit still remains controversial and gives rise to a renewed interest. The focus of the issues is whether these quantum properties have a conventional bulk nature or just the surface effect due to the significant spin-orbital interaction and in relation to the Bi-based topological insulators. Here, we present angular-dependent magnetoresistance (AMR) measurements on single-crystal bismuth nanoribbons of different thickness with magnetic fields up to 31 T. In thin nanoribbons with thickness of ~40 nm, a two-fold rational symmetry of the low field AMR spectra and two sets of 1/2-shifted (i.e. {γ}=1/2) Shubnikov-de Haas (SdH) quantum oscillations with exact two- dimensional (2D) character were obtained. However, when the thickness of the ribbon increases, a 3D bulk-like SdH oscillations with {γ}=0 and a four-fold rotational symmetry of the AMR spectra appear. These results unambiguously provided the first transport evidence of the topological 2D metallic surface states in thinner nanoribbons with an insulating bulk. Our observations provide a promising pathway to understand the quantum phenomena in Bi arising from the surface states. ; Comment: Accepted by ACS Nano