In-situ characterization and assessment of arsenic (As) mobility in sediments was scarce. In this study, the distributions of labile As at a vertical resolution of 2 mm were obtained in the sediments of a large Lake Taihu through in-situ measurements using a Zr-oxide diffusive gradients in thin films (Zr-oxide DGT) technique. The DGT-labile As, interpreted as DGT flux (F-DGT), exhibited three different patterns in the lake, with all the patterns generally showing an increasing mobility followed by a decreasing mobility with sediment depth. The mobility of As could be characterized by the average F-DGT (0.06-1.27 pg cm(-2) s(-1)) in the top 10 mm surface sediments, the maximal FDGT (FDGT-M, 0.14-2.44 pg cm(-2) s(-1)) in the end of the initial increasing phase of F-DGT, and the diffusion length (Delta L, 28 -66 mm) from the depth showing the FDGT-M to the sediment-water interface. The upward mobilization of labile As from the deep sediments to the surface sediments and overlying water became evident when FDGT-M > 1.7 pg cm(-2) s(-1) or Delta L < 41 mm. The results, for the first time, showed a prospect in in-situ risk assessment of the pollution of sediment As. It was suggested that the increasing mobility of As in the upper sediments was controlled by the reduction of As(V) and the reductive dissolution of Fe(III) (hydr) oxides, while the decreasing mobility in the deep sediments was attributed to immobilization of As(III) by secondary Fe(II)-bearing minerals. (C) 2016 Elsevier Ltd. All rights reserved.