The reflectance of wheat's canopy exhibits angular sensitivity, which can influence the accuracy of different methods for its leaf area index (LAI) estimation through multi-angular remote sensing. The primary objective of this study was to assess and compare the ability of various methods for LAI estimation from 13 view zenith angles (VZAs). The four methods included: (1) common hyper-spectral vegetation indices (VIs), (2) optimal two-band combination VIs (i.e., VIs: normalized difference index, simple ratio index, and difference vegetation index), (3) back-propagation neural network (BPNN), and (4) partial least squares regression (PLSR). Our results demonstrated that the red-edge plays a key role in estimating LAI, in that the traditional VIs, optimal two-band VIs, and PLSR including the red-edge band all showed satisfactory performance, with coefficient of determination (R2) > 0.72 in the nadir direction. However, the estimation accuracy of LAI was not positively related with band number, and BPNN gave unsatisfactory results under a larger viewing angle, with R2 ≤ 0.60 for extreme angles. The predictive ability of all four methods declined with an increasing VZA, with reliable LAI estimation near the nadir direction. Importantly, by comparing the four methods, PLSR emerged as superior in both its estimation accuracy and angular insensitivity, with R2 = 0.83 in the nadir direction and ≥ 0.65 for extreme angles. For this reason, we highly recommend it be used with multi-angular remote sensing data, especially in agricultural applications.