Remote sensing technology is a timely and cost-efficient method for leaf area index (LAI) estimation, especially for less accessible areas such as mangrove forests. Confounded by the poor penetrability of optical images, most previous studies focused on estimating the LAI of the main canopy, ignoring the impact of the understory. This study investigated the capability of multispectral Sentinel-2 (S2) imagery, airborne hyperspectral imagery (HSI), and airborne LiDAR data for overstory (OLe) and understory (ULe) LAI estimation of a multi-layered mangrove stand in the Mai Po, Hong Kong. The LAI of overstory and understory mangroves was measured using digital hemispherical photography (DHP) in the field to calculate the OLe and ULe. LiDAR data was employed to stratify the overstory and understory. Vegetation indices (VIs) and LiDAR metrics were generated as predictors to build regression models against the OLe and ULe with multiple parametric and non-parametric methods. The OLe model fitting results were typically better than ULe because of the dominant contribution of the overstory to the remotely sensed signal. Single red edge VI derived from HSI data delivered the low RMSE = 0.12 and high R2adj = 0.79 for OLe model fitting. The synergetic use LiDAR metrics and S2 VIs performed best for ULe model fitting with RMSE = 0.33, R2adj = 0.84. OLe estimation benefited from the high spatial and spectral resolution HSI that was found less confounded by the understory. Apart from penetration attribute, LiDAR data could separately describe the upper and lower canopy, which reduced the noise from other components, thereby improving the ULe estimation.