Optical remote sensing indices play an important role in vegetation information extraction and have been widely serving ecology, agriculture and forestry, urban monitoring, and other communities. Remote sensing indices are constructed from individual bands depending on special characteristics to enhance the typical spectral features for the identification or distinction of surface land covers. With the development of quantitative remote sensing, there is a rapidly increasing requirement for accurate data processing and modeling. It is well known that the geometry-induced variation observed on surface reflectance is not ignorable, but the situation of uncertainty thereby introduced into these indices still needs further detailed understanding. We adopted the ground multi-angle hyperspectrum, spectral response function (SRF) of Thematic Mapper (TM), Enhanced Thematic Mapper (ETM+), Operational Land Imager (OLI), Moderate-Resolution Imaging Spectroradiometer (MODIS), and Multi-Spectral Instrument (MSI) optical sensors and simulated their sensor-like spectral reflectance; then, we investigated the potential angle effect uncertainty on optical indices that have been frequently involved in vegetation monitoring and examined the forward/backward effect over both the ground-based level and the actual Landsat TM/ETM+ overlapped region. Our results on the discussed indices and sensors show the following: (1) Identifiable angle effects exist with a more elevated influence than that introduced by band difference among sensors; (2) The absolute difference of forward and backward direction can reach up to −0.03 to 0.1 within bands of the TM/ETM+ overlapped region; (3) The investigation at ground level indicates that there are different variations of angle effect transmitted to each remote sensing index. Regarding cases of crop canopy at various growth phases, most of the discussed indices have more than a 20% relative difference in nadir value except Normalized Difference Vegetation Index (NDVI) and Normalized Difference Water Index (NDWI), at less than 10%, and Normalized Burn Ratio (NBR) at less than 16%. For the case of wax maturity stage, the relative difference in nadir value of Enhanced Vegetation Index (EVI), Soil-Adjusted Vegetation Index (SAVI), Ratio Vegetation Index (RVI), Char Soil Index (CSI), NBR, Normalized Difference Moisture Index (NDMI), and SWIR2/NIR exceeded 50%, among which the values for NBR and NDMI reached up to 115.8% and 206.7%, respectively; (4) Various schemes of index construction imply different developments of angle effect uncertainty. The “difference” indices can partially suppress the directional influence, while the “ratio” indices show high potential to amplify the angle effect. This study reveals that the angle-induced uncertainty of these indices is greater than that induced by the spectrum mismatch among sensors, especially under the senescence period. In addition, based on this work, indices with a suppressed potential of angle effect are recommended for vegetation monitoring or information retrieval to avoid unexpected effects.