We investigate the superconducting-gap anisotropy in one of the recently discovered BiS2-based superconductors, NdO0.71F0.29BiS2 (Tc ∼ 5 K), using laser-based angle-resolved photoemission spectroscopy. Whereas the previously discovered high-Tc superconductors such as copper oxides and iron-based superconductors, which are believed to have unconventional superconducting mechanisms, have 3d electrons in their conduction bands, the conduction band of BiS2-based superconductors mainly consists of Bi 6p electrons, and hence the conventional superconducting mechanism might be expected. Contrary to this expectation, we observe a strongly anisotropic superconducting gap. This result strongly suggests that the pairing mechanism for NdO0.71F0.29BiS2 is unconventional one and we attribute the observed anisotropy to competitive or cooperative multiple paring interactions.