Leaf area index (LAI) is a key parameter in plant growth monitoring. For several decades, vegetation indices-based empirical method has been widely-accepted in LAI retrieval. A growing number of spectral indices have been proposed to tailor LAI estimations, however, saturation effect has long been an obstacle. In this paper, we classify the selected 14 vegetation indices into five groups according to their characteristics. In this study, we proposed a new index for LAI retrieval-transformed triangular vegetation index (TTVI), which replaces NIR and red bands of triangular vegetation index (TVI) into NIR and red-edge bands. All fifteen indices were calculated and analyzed with both hyperspectral and multispectral data. Best-fit models and k-fold cross-validation were conducted. The results showed that TTVI performed the best predictive power of LAI for both hyperspectral and multispectral data, and mitigated the saturation effect. The R2 and RMSE values were 0.60, 1.12; 0.59, 1.15, respectively. Besides, TTVI showed high estimation accuracy for sparse (LAI < 4) and dense canopies (LAI > 4). Our study provided the value of the Red-edge bands of the Sentinel-2 satellite sensors in crop LAI retrieval, and demonstrated that the new index TTVI is applicable to inverse LAI for both low-to-moderate and moderate-to-high vegetation cover.